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Ammonia (NH3) is the major alkaline species in the atmosphere and plays an important role in aerosol formation, which affects local air quality and the radiation budget. NH3 in the upper troposphere and lower stratosphere (UTLS) is difficult to detect, and only limited observations are available. We present two-dimensional trace gas measurements of NH3 obtained by the airborne infrared imaging limb sounder GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) that was operated on board the research aircraft Geophysica within the Asian monsoon anticyclone during the StratoClim campaign (July 2017) and on board HALO (the High Altitude and LOng Range research aircraft) above the South Atlantic during the SouthTRAC campaign (September–November 2019). We compare these GLORIA measurements in the UTLS with results of the CAMS (Copernicus Atmosphere Monitoring Service) reanalysis and forecast model to evaluate its performance. The GLORIA observations reveal large enhancements of NH3 of more than 1 ppbv in the Asian monsoon upper troposphere but no clear indication of NH3 in biomass burning plumes in the upper troposphere above the South Atlantic above the instrument's detection limit of around 20 pptv. In contrast, CAMS reanalysis and forecast simulation results indicate strong enhancements of NH3 in both measured scenarios. Comparisons of other retrieved pollution gases, such as peroxyacetyl nitrate (PAN), show the ability of CAMS models to generally reproduce the biomass burning plumes above the South Atlantic. However, NH3 concentrations are largely overestimated by the CAMS models within these plumes. We suggest that emission strengths used by CAMS models are of lower accuracy for biomass burning in comparison to agricultural sources in the Asian monsoon. Further, we suggest that loss processes of NH3 during transport to the upper troposphere may be underestimated for the biomass burning cases above the South Atlantic. Since NH3 is strongly undersampled, in particular at higher altitudes, we hope for regular vertically resolved measurements of NH3 from the proposed CAIRT (Changing-Atmosphere Infra-Red Tomography Explorer) mission to strengthen our understanding of this important trace gas in the atmosphere.

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.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an infrared imaging FTS (Fourier transform spectrometer) with a 2-D infrared detector that is operated on two high-flying research aircraft. It has flown on eight campaigns and measured along more than 300 000 km of flight track. This paper details our instrument calibration and characterization efforts, which, in particular, almost exclusively leverage in-flight data. First, we present the framework of our new calibration scheme, which uses information from all three available calibration sources (two blackbodies and upward-pointing “deep space” measurements). Part of this scheme is a new algorithm for correcting the erratically changing nonlinearity of a subset of detector pixels and the identification of the remaining bad pixels. Using this new calibration, we derive a 1σ bound of 1 % on the instrument gain error and a bound of 30 nW cm−2 sr−1 cm on the instrument offset error. We show how we can examine the noise and spectral accuracy for all measured atmospheric spectra and derive a spectral accuracy of 5 ppm on average. All these errors are compliant with the initial instrument requirements. We also discuss, for the first time, the pointing system of the GLORIA instrument. Combining laboratory calibration efforts with the measurement of astronomical bodies during the flight, we can achieve a pointing accuracy of 0.032∘, which corresponds to one detector pixel. The paper concludes with a brief study of how these newly characterized instrument parameters affect temperature and ozone retrievals. We find that the pointing uncertainty and, to a lesser extent, the instrument gain uncertainty are the main contributors to the error in the result.

In this study, we present simultaneous airborne measurements of peroxyacetyl nitrate (PAN), ethane (C2H6), formic acid (HCOOH), methanol (CH3OH), and ethylene (C2H4) above the South Atlantic in September and October 2019. Observations were obtained from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA), as two-dimensional altitude cross sections along the flight path. The flights were part of the SouthTRAC (Transport and Composition in the Southern Hemisphere Upper Troposphere/Lower Stratosphere) campaign with the German High Altitude and Long Range Research Aircraft (HALO). On two flights (8 September 2019 and 7 October 2019), large enhancements of all these substances were found between 7 and 14 km altitude with maximum volume mixing ratios (VMRs) of 1000 pptv for PAN, 1400 pptv for C2H6, 800 pptv for HCOOH, 4500 pptv for CH3OH, and 200 pptv for C2H4. One flight showed a common filamentary structure in the trace gas distributions, while the second flight is characterized by one large plume. Using backward trajectories, we show that measured pollutants likely reached upper troposphere and lower stratosphere (UTLS) altitudes above South America and central Africa, where elevated PAN VMRs are visible at the surface layer of the Copernicus Atmosphere Monitoring Service (CAMS) model during the weeks before both measurements. In comparison to results of the CAMS reanalysis interpolated onto the GLORIA measurement geolocations, we show that the model is able to reproduce the overall structure of the measured pollution trace gas distributions. For PAN, the absolute VMRs are in agreement with the GLORIA measurements. However, C2H6 and HCOOH are generally underestimated by the model, while CH3OH and C2H4, the species with the shortest atmospheric lifetimes of the pollution trace gases discussed, are overestimated by CAMS. The good agreement between model and observations for PAN suggests that the general transport pathways and emissions locations are well captured by the model. The poorer agreement for other species is therefore most likely linked to model deficiencies in the representation of loss processes and emission strength.

Water vapour and ozone are important for the thermal and radiative balance of the upper troposphere (UT) and lowermost stratosphere (LMS). Both species are modulated by transport processes. Chemical and microphysical processes affect them differently. Thus, representing the different processes and their interactions is a challenging task for dynamical cores, chemical modules and microphysical parameterisations of state-of-the-art atmospheric model components. To test and improve the models, high-resolution measurements of the UT–LMS are required. Here, we use measurements taken in a flight of the GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) instrument on HALO (High Altitude and LOng Range Research Aircraft). The German research aircraft HALO performed a research flight on 26 February 2016 that covered deeply subsided air masses of the aged 2015/16 Arctic vortex, high-latitude LMS air masses, a highly textured region affected by troposphere-to-stratosphere exchange and high-altitude cirrus clouds. Therefore, it provides a challenging multifaceted case study for comparing GLORIA observations with state-of-the-art atmospheric model simulations in a complex UT–LMS region at a late stage of the Arctic winter 2015/16. Using GLORIA observations in this manifold scenario, we test the ability of the numerical weather prediction (NWP) model ICON (ICOsahedral Nonhydrostatic) with the extension ART (Aerosols and Reactive Trace gases) and the chemistry–climate model (CCM) EMAC (ECHAM5/MESSy Atmospheric Chemistry – fifth-generation European Centre Hamburg general circulation model/Modular Earth Submodel System) to model the UT–LMS composition of water vapour (H2O), ozone (O3), nitric acid (HNO3) and clouds. Within the scales resolved by the respective model, we find good overall agreement of both models with GLORIA. The applied high-resolution ICON-ART set-up involving an R2B7 nest (local grid refinement with a horizontal resolution of about 20 km), covering the HALO flight region, reproduces mesoscale dynamical structures well. Narrow moist filaments in the LMS observed by GLORIA at tropopause gradients in the context of a Rossby wave breaking event and in the vicinity of an occluded Icelandic low are clearly reproduced by the model. Using ICON-ART, we show that a larger filament in the west was transported horizontally into the Arctic LMS in connection with a jet stream split associated with poleward breaking of a cyclonically sheared Rossby wave. Further weaker filaments are associated with an older tropopause fold in the east. Given the lower resolution (T106) of the nudged simulation of the EMAC model, we find that this model also reproduces these features well. Overall, trace gas mixing ratios simulated by both models are in a realistic range, and major cloud systems observed by GLORIA are mostly reproduced. However, we find both models to be affected by a well-known systematic moist bias in the LMS. Further biases are diagnosed in the ICON-ART O3, EMAC H2O and EMAC HNO3 distributions. Finally, we use sensitivity simulations to investigate (i) short-term cirrus cloud impacts on the H2O distribution (ICON-ART), (ii) the overall impact of polar winter chemistry and microphysical processing on O3 and HNO3 (ICON-ART and EMAC), (iii) the impact of the model resolution on simulated parameters (EMAC), and (iv) consequences of scavenging processes by cloud particles (EMAC). We find that changing the horizontal model resolution results in notable systematic changes for all species in the LMS, while scavenging processes play a role only in the case of HNO3. We discuss the model biases and deficits found in this case study that potentially affect forecasts and projections (adversely) and provide suggestions for further model improvements.

To better understand the impact of gravity waves (GWs) on the middle atmosphere in the current and future climate, it is essential to understand their excitation mechanisms and to quantify their basic properties. Here a new process for GW excitation by orography–jet interaction is discussed. In a case study, we identify the source of a GW observed over Greenland on 10 March 2016 during the POLSTRACC (POLar STRAtosphere in a Changing Climate) aircraft campaign. Measurements were taken with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) instrument deployed on the High Altitude Long Range (HALO) German research aircraft. The measured infrared limb radiances are converted into a 3D observational temperature field through the use of inverse modelling and limited-angle tomography. We observe GWs along a transect through Greenland where the GW packet covers ≈ 1/3 of the Greenland mainland. GLORIA observations indicate GWs between 10 and 13 km of altitude with a horizontal wavelength of 330 km, a vertical wavelength of 2 km and a large temperature amplitude of 4.5 K. Slanted phase fronts indicate intrinsic propagation against the wind, while the ground-based propagation is with the wind. The GWs are arrested below a critical layer above the tropospheric jet. Compared to its intrinsic horizontal group velocity (25–72 m s−1) the GW packet has a slow vertical group velocity of 0.05–0.2 m s−1. This causes the GW packet to propagate long distances while spreading over a large area and remaining constrained to a narrow vertical layer. A plausible source is not only orography, but also out-of-balance winds in a jet exit region and wind shear. To identify the GW source, 3D GLORIA observations are combined with a gravity wave ray tracer, ERA5 reanalysis and high-resolution numerical experiments. In a numerical experiment with a smoothed orography, GW activity is quite weak, indicating that the GWs in the realistic orography experiment are due to orography. However, analysis shows that these GWs are not mountain waves. A favourable area for spontaneous GW emission is identified in the jet by the cross-stream ageostrophic wind, which indicates when the flow is out of geostrophic balance. Backwards ray-tracing experiments trace into the jet and regions where the Coriolis and the pressure gradient forces are out of balance. The difference between the full and a smooth-orography experiment is investigated to reveal the missing connection between orography and the out-of-balance jet. We find that this is flow over a broad area of elevated terrain which causes compression of air above Greenland. The orography modifies the wind flow over large horizontal and vertical scales, resulting in out-of-balance geostrophic components. The out-of-balance jet then excites GWs in order to bring the flow back into balance. This is the first observational evidence of GW generation by such an orography–jet mechanism.

This paper presents measurements of ozone, water vapour and nitric acid (HNO3) in the upper troposphere/lower stratosphere (UTLS) over North Atlantic and Europe. The measurements were acquired with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the Wave Driven Isentropic Exchange (WISE) campaign in October 2017. GLORIA is an airborne limb imager capable of acquiring both 2-D data sets (curtains along the flight path) and, when the carrier aircraft is flying around the observed air mass, spatially highly resolved 3-D tomographic data. Here, we present a case study of a Rossby wave (RW) breaking event observed during two subsequent flights 2 d apart. RW breaking is known to steepen tracer gradients and facilitate stratosphere–troposphere exchange (STE). Our measurements reveal complex spatial structures in stratospheric tracers (ozone and nitric acid) with multiple vertically stacked filaments. Backward-trajectory analysis is used to demonstrate that these features are related to several previous Rossby wave breaking events and that the small-scale structure of the UTLS in the Rossby wave breaking region, which is otherwise very hard to observe, can be understood as stirring and mixing of air masses of tropospheric and stratospheric origin. It is also shown that a strong nitric acid enhancement observed just above the tropopause is likely a result of NOx production by lightning activity. The measurements showed signatures of enhanced mixing between stratospheric and tropospheric air near the polar jet with some transport of water vapour into the stratosphere. Some of the air masses seen in 3-D data were encountered again 2 d later, stretched to very thin filament (horizontal thickness down to 30 km at some altitudes) rich in stratospheric tracers. This repeated measurement allowed us to directly observe and analyse the progress of mixing processes in a thin filament over 2 d. Our results provide direct insight into small-scale dynamics of the UTLS in the Rossby wave breaking region, which is of great importance to understanding STE and poleward transport in the UTLS.

Measurements of the pollution trace gases ethane (C2H6), ethyne (C2H2), formic acid (HCOOH), and peroxyacetyl nitrate (PAN) were performed in the North Atlantic upper troposphere and lowermost stratosphere (UTLS) region with the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) with high spatial resolution down to cloud top. Observations were made during flights with the German research aircraft HALO (High Altitude and LOng Range Research Aircraft) in the frame of the WISE (Wave-driven ISentropic Exchange) campaign, which was carried out in autumn 2017 from Shannon (Ireland) and Oberpfaffenhofen (Germany). Enhanced volume mixing ratios (VMRs) of up to 2.2 ppbv C2H6, 0.2 ppbv C2H2, 0.9 ppbv HCOOH, and 0.4 ppbv PAN were detected during the flight on 13 September 2017 in the upper troposphere and around the tropopause above the British Isles. Elevated quantities of PAN were measured even in the lowermost stratosphere (locally up to 14 km), likely reflecting the fact that this molecule has the longest lifetime of the four species discussed herein. Backward trajectory calculations as well as global three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS) simulations with artificial tracers of air mass origin have shown that the main sources of the observed pollutant species are forest fires in North America and anthropogenic pollution in South Asia and Southeast Asia uplifted and moved within the Asian monsoon anticyclone (AMA) circulation system. After release from the AMA, these species or their precursor substances are transported by strong tropospheric winds over large distances, depending on their particular atmospheric lifetime of up to months. Observations are compared to simulations with the atmospheric models EMAC (ECHAM5/MESSy Atmospheric Chemistry) and CAMS (Copernicus Atmosphere Monitoring Service). These models are qualitatively able to reproduce the measured VMR enhancements but underestimate the absolute amount of the increase. Increasing the emissions in EMAC by a factor of 2 reduces the disagreement between simulated and measured results and illustrates the importance of the quality of emission databases used in chemical models.

Numerical weather forecast systems like the ECMWF IFS (European Centre for Medium-Range Weather Forecasts – Integrated Forecasting System) are known to be affected by a moist bias in the extratropical lowermost stratosphere (LMS) which results in a systematic cold bias there. We use high-spatial-resolution water vapor measurements by the airborne infrared limb-imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) during the PGS (POLSTRACC/GW-LCYCLE-II/SALSA) campaign to study the LMS moist bias in ECMWF analyses and 12 h forecasts from January to March 2016. Thereby, we exploit the two-dimensional observational capabilities of GLORIA, when compared to in situ observations, and the higher vertical and horizontal resolution, when compared to satellite observations. Using GLORIA observations taken during five flights in the polar sub-vortex region around Scandinavia and Greenland, we diagnose a systematic moist bias in the LMS exceeding +50 % (January) to +30 % (March) at potential vorticity levels from 10 PVU (∼ highest level accessed with suitable coverage) to 7 PVU. In the diagnosed time period, the moist bias decreases at the highest and driest air masses observed but clearly persists at lower levels until mid-March. Sensitivity experiments with more frequent temporal output, and lower or higher horizontal and vertical resolution, show the short-term forecasts to be practically insensitive to these parameters on timescales of < 12 h. Our results confirm that the diagnosed moist bias is already present in the initial conditions (i.e., the analysis) and thus support the hypothesis that the cold bias develops as a result of forecast initialization. The moist bias in the analysis might be explained by a model bias together with the lack of water vapor observations suitable for assimilation above the tropopause.

We present the first high-resolution measurements of pollutant trace gases in the Asian summer monsoon upper troposphere and lowermost stratosphere (UTLS) from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign based in Kathmandu, Nepal, 2017. Measurements of peroxyacetyl nitrate (PAN), acetylene (C2H2), and formic acid (HCOOH) show strong local enhancements up to altitudes of 16 km. More than 500 pptv of PAN, more than 200 pptv of C2H2, and more than 200 pptv of HCOOH are observed. Air masses with increased volume mixing ratios of PAN and C2H2 at altitudes up to 18 km, reaching to the lowermost stratosphere, were present at these altitudes for more than 10 d, as indicated by trajectory analysis. A local minimum of HCOOH is correlated with a previously reported maximum of ammonia (NH3), which suggests different washout efficiencies of these species in the same air masses. A backward trajectory analysis based on the models Alfred Wegener InsTitute LAgrangian Chemistry/Transport System (ATLAS) and TRACZILLA, using advanced techniques for detection of convective events, and starting at geolocations of GLORIA measurements with enhanced pollution trace gas concentrations, has been performed. The analysis shows that convective events along trajectories leading to GLORIA measurements with enhanced pollutants are located close to regions where satellite measurements by the Ozone Monitoring Instrument (OMI) indicate enhanced tropospheric columns of nitrogen dioxide (NO2) in the days prior to the observation. A comparison to the global atmospheric models Copernicus Atmosphere Monitoring Service (CAMS) and ECHAM/MESSy Atmospheric Chemistry (EMAC) has been performed. It is shown that these models are able to reproduce large-scale structures of the pollution trace gas distributions for one part of the flight, while the other part of the flight reveals large discrepancies between models and measurement. These discrepancies possibly result from convective events that are not resolved or parameterized in the models, uncertainties in the emissions of source gases, and uncertainties in the rate constants of chemical reactions.

The Arctic winter 2015–2016 was characterized by exceptionally low stratospheric temperatures, favouring the formation of polar stratospheric clouds (PSCs) from mid-December until the end of February down to low stratospheric altitudes. Observations by GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) on HALO (High Altitude and LOng range research aircraft) during the PGS (POLSTRACC–GW-LCYCLE II–SALSA) campaign from December 2015 to March 2016 allow the investigation of the influence of denitrification on the lowermost stratosphere (LMS) with a high spatial resolution. Two-dimensional vertical cross sections of nitric acid (HNO3) along the flight track and tracer–tracer correlations derived from the GLORIA observations document detailed pictures of wide-spread nitrification of the Arctic LMS during the course of an entire winter. GLORIA observations show large-scale structures and local fine structures with enhanced absolute HNO3 volume mixing ratios reaching up to 11 ppbv at altitudes of 13 km in January and nitrified filaments persisting until the middle of March. Narrow coherent structures tilted with altitude of enhanced HNO3, observed in mid-January, are interpreted as regions recently nitrified by sublimating HNO3-containing particles. Overall, extensive nitrification of the LMS between 5.0 and 7.0 ppbv at potential temperature levels between 350 and 380 K is estimated. The GLORIA observations are compared with CLaMS (Chemical Lagrangian Model of the Stratosphere) simulations. The fundamental structures observed by GLORIA are well reproduced, but differences in the fine structures are diagnosed. Further, CLaMS predominantly underestimates the spatial extent of HNO3 maxima derived from the GLORIA observations as well as the overall nitrification of the LMS. Sensitivity simulations with CLaMS including (i) enhanced sedimentation rates in case of ice supersaturation (to resemble ice nucleation on nitric acid trihydrate (NAT)), (ii) a global temperature offset, (iii) modified growth rates (to resemble aspherical particles with larger surfaces) and (iv) temperature fluctuations (to resemble the impact of small-scale mountain waves) slightly improved the agreement with the GLORIA observations of individual flights. However, no parameter could be isolated which resulted in a general improvement for all flights. Still, the sensitivity simulations suggest that details of particle microphysics play a significant role for simulated LMS nitrification in January, while air subsidence, transport and mixing become increasingly important for the simulated HNO3 distributions towards the end of the winter.

The Arctic winter 2015/16 was characterized by cold stratospheric temperatures. Here we present a comprehensive view of the temporal evolution of chlorine in the lowermost stratosphere over the course of the studied winter. We utilize two-dimensional vertical cross sections of ozone (O3) and chlorine nitrate (ClONO2), measured by the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) during the POLSTRACC/GW-LCYCLE II/GWEX/SALSA campaigns, to investigate the tropopause region in detail. Observations from three long-distance flights in January, February, and March 2016 are discussed. ClONO2 volume mixing ratios up to 1100 pptv were measured at 380 K potential temperature in mesoscale structures. Similar mesoscale structures are also visible in O3 measurements. Both trace gas measurements are applied to evaluate simulation results from the chemistry transport model CLaMS (Chemical Lagrangian Model of the Stratosphere) and the chemistry–climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry). These comparisons show agreement within the expected performance of these models. Satellite measurements from Aura/MLS (Microwave Limb Sounder) and SCISAT/ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) provide an overview over the whole winter and information about the stratospheric situation above the flight altitude. Time series of these satellite measurements reveal unusually low hydrochloric acid (HCl) and ClONO2 at 380 K from the beginning of January to the end of February 2016, while chlorine monoxide (ClO) is strongly enhanced. In March 2016, unusually rapid chlorine deactivation into HCl is observed instead of deactivation into ClONO2, the more typical pathway for deactivation in the Arctic. Chlorine deactivation observed in the satellite time series is well reproduced by CLaMS. Sensitivity simulations with CLaMS demonstrate the influence of low abundances of O3 and reactive nitrogen (NOy) due to ozone depletion and sedimentation of NOy-containing particles, respectively. On the basis of the different altitude and time ranges of these effects, we conclude that the substantial chlorine deactivation into HCl at 380 K arose as a result of very low ozone abundances together with low temperatures. Additionally, CLaMS estimates ozone depletion of at least 0.4 ppmv at 380 K and 1.75 ppmv at 490 K, which is comparable to other extremely cold Arctic winters. We have used CLaMS trajectories to analyze the history of enhanced ClONO2 measured by GLORIA. In February, most of the enhanced ClONO2 is traced back to chlorine deactivation that had occurred within the past few days prior to the GLORIA measurement. In March, after the final warming, air masses in which chlorine has previously been deactivated into ClONO2 have been transported in the remnants of the polar vortex towards the location of measurement for at least 11 d.

We report airborne remote-sensing observations of a tropopause fold during two crossings of the polar front jet over northern Italy on 12 January 2016. The GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) observations allowed for a simultaneous mapping of temperature, water vapour, and ozone. They revealed deep, dry, and ozone-rich intrusions into the troposphere. The mesoscale fine structures of dry filaments at the cyclonic shear side north of the jet and tongues of moist air entraining tropospheric air into the stratosphere along the anticyclonic shear side south of the jet were clearly resolved by GLORIA observations. Vertically propagating mountain waves with recorded temperature residuals exceeding ±3 K were detected above the Apennines. Their presence enhanced gradients of all variables locally in the vicinity of the tropopause. The combination of H2O − O3 correlations with potential temperature reveals an active mixing region and shows clear evidence of troposphere-to-stratosphere and stratosphere-to-troposphere exchange. High-resolution short-term deterministic forecasts of ECMWF's integrated forecast system (IFS) applying GLORIA's observational filter reproduce location, shape, and depth of the tropopause fold very well. The fine structure of the mixing region, however, cannot be reproduced even with the 9 km horizontal resolution of the IFS, used here. This case study demonstrates convincingly the capabilities of linear limb-imaging observations to resolve mesoscale fine structures in the upper troposphere and lower stratosphere, validates the high quality of the IFS data, and suggests that mountain wave perturbations have the potential to modulate exchange processes in the vicinity of tropopause folds.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) was operated on board the German High Altitude and Long Range Research Aircraft (HALO) during the PGS (POLSTRACC/GW-LCYCLE/SALSA) aircraft campaigns in the Arctic winter 2015/2016. Research flights were conducted from 17 December 2015 until 18 March 2016 within 25–87° N, 80° W–30° E. From the GLORIA infrared limb-emission measurements, two-dimensional cross sections of temperature, HNO3, O3, ClONO2, H2O and CFC-12 are retrieved. During 15 scientific flights of the PGS campaigns the GLORIA instrument measured more than 15 000 atmospheric profiles at high spectral resolution. Dependent on flight altitude and tropospheric cloud cover, the profiles retrieved from the measurements typically range between 5 and 14 km, and vertical resolutions between 400 and 1000 m are achieved. The estimated total (random and systematic) 1σ errors are in the range of 1 to 2 K for temperature and 10 % to 20 % relative error for the discussed trace gases. Comparisons to in situ instruments deployed on board HALO have been performed. Over all flights of this campaign the median differences and median absolute deviations between in situ and GLORIA observations are −0.75 K ± 0.88 K for temperature, −0.03 ppbv ± 0.85 ppbv for HNO3, −3.5 ppbv ± 116.8 ppbv for O3, −15.4 pptv ± 102.8 pptv for ClONO2, −0.13 ppmv ± 0.63 ppmv for H2O and −19.8 pptv ± 46.9 pptv for CFC-12. Seventy-three percent of these differences are within twice the combined estimated errors of the cross-compared instruments. Events with larger deviations are explained by atmospheric variability and different sampling characteristics of the instruments. Additionally, comparisons of GLORIA HNO3 and O3 with measurements of the Aura Microwave Limb Sounder (MLS) instrument show highly consistent structures in trace gas distributions and illustrate the potential of the high-spectral-resolution limb-imaging GLORIA observations for resolving narrow mesoscale structures in the upper troposphere and lower stratosphere (UTLS).

Atmospheric gravity waves are a major cause of uncertainty in atmosphere general circulation models. This uncertainty affects regional climate projections and seasonal weather predictions. Improving the representation of gravity waves in general circulation models is therefore of primary interest. In this regard, measurements providing an accurate 3-D characterization of gravity waves are needed. Using the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA), the first airborne implementation of a novel infrared limb imaging technique, a gravity wave event over Iceland was observed. An air volume disturbed by this gravity wave was investigated from different angles by encircling the volume with a closed flight pattern. Using a tomographic retrieval approach, the measurements of this air mass at different angles allowed for a 3-D reconstruction of the temperature and trace gas structure. The temperature measurements were used to derive gravity wave amplitudes, 3-D wave vectors, and direction-resolved momentum fluxes. These parameters facilitated the backtracing of the waves to their sources on the southern coast of Iceland. Two wave packets are distinguished, one stemming from the main mountain ridge in the south of Iceland and the other from the smaller mountains in the north. The total area-integrated fluxes of these two wave packets are determined. Forward ray tracing reveals that the waves propagate laterally more than 2000 km away from their source region. A comparison of a 3-D ray-tracing version to solely column-based propagation showed that lateral propagation can help the waves to avoid critical layers and propagate to higher altitudes. Thus, the implementation of oblique gravity wave propagation into general circulation models may improve their predictive skills.

The first stratospheric measurements of the diurnal variation in the inorganic bromine (Bry) reservoir species BrONO2 around sunrise and sunset are reported. Arctic flights of the balloon-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) were carried out from Kiruna (68° N, Sweden) in January 2010 and March 2011 inside the stratospheric polar vortices where diurnal variations of BrONO2 around sunrise have been observed. High nighttime BrONO2 volume mixing ratios of up to 21 pptv (parts per trillion by volume) were detected in late winter 2011 in the absence of polar stratospheric clouds (PSCs). In contrast, the amount of measured BrONO2 was significantly lower in January 2010 due to low available NO2 amounts (for the build-up of BrONO2), the heterogeneous destruction of BrONO2 on PSC particles, and the gas-phase interaction of BrO (the source to form BrONO2) with ClO. A further balloon flight took place at midlatitudes from Timmins (49° N, Canada) in September 2014. Mean BrONO2 mixing ratios of 22 pptv were observed after sunset in the altitude region between 21 and 29 km. Measurements are compared and discussed with the results of a multi-year simulation performed with the chemistry climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). The calculated temporal variation in BrONO2 largely reproduces the balloon-borne observations. Using the nighttime simulated ratio between BrONO2 and Bry, the amount of Bry observed by MIPAS-B was estimated to be about 21–25 pptv in the lower stratosphere.

The Geostationary Emission Explorer for Europe (G3E) is a concept for a geostationary satellite sounder that aims to constrain the sources and sinks of greenhouse gases carbon dioxide (CO2) and methane (CH4) for continental-scale regions. Its primary focus is on central Europe. G3E carries a spectrometer system that collects sunlight backscattered from the Earth's surface and atmosphere in the near-infrared (NIR) and shortwave-infrared (SWIR) spectral range. Solar absorption spectra allow for spatiotemporally dense observations of the column-average concentrations of carbon dioxide (XCO2), methane (XCH4), and carbon monoxide (XCO). The mission concept in particular facilitates sampling of the diurnal variation with several measurements per day during summer. Here, we present the mission concept and carry out an initial performance assessment of the retrieval capabilities. The radiometric performance of the 4 grating spectrometers is tuned to reconcile small ground-pixel sizes (~2 km × 3 km at 50° latitude) with short single-shot exposures (~2.9 s) that allow for sampling continental regions such as central Europe within 2 h while providing a sufficient signal-to-noise ratio. The noise errors to be expected for XCO2, XCH4, and XCO are assessed through retrieval simulations for a European trial ensemble. Generally, single-shot precision for the targeted XCO2 and XCH4 is better than 0.5 % with some exception for scenes with low infrared surface albedo observed under low sun conditions in winter. For XCO, precision is generally better than 10 %. Performance for aerosol and cirrus loaded atmospheres is assessed by mimicking G3E's slant view on Europe for an ensemble of atmospheric scattering properties used previously for evaluating nadir-viewing low-Earth-orbit (LEO) satellites. While retrieval concepts developed for LEO configurations generally succeed in mitigating aerosol- and cirrus-induced retrieval errors for G3E's setup, residual errors are somewhat greater in geostationary orbit (GEO) than in LEO. G3E's deployment in the vicinity of the Meteosat Third Generation (MTG) satellites has the potential to make synergistic use of MTG's sounding capabilities e.g. with respect to characterization of aerosol and cloud properties or with respect to enhancing carbon monoxide retrievals by combining G3E's solar and MTG's thermal infrared spectra.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) presents new opportunities for the retrieval of trace gases in the upper troposphere and lower stratosphere. The radiometric calibration of the measured signal is achieved using in-flight measurements of reference blackbody and upward-pointing "deep space" scenes. In this paper, we present techniques developed specifically to calibrate GLORIA data exploiting the instrument's imaging capability. The algorithms discussed here make use of the spatial correlation of parameters across GLORIA's detector pixels in order to mitigate the noise levels and artefacts in the calibration measurements. This is achieved by combining a priori and empirical knowledge about the instrument background radiation with noise-mitigating compression methods, specifically low-pass filtering and principal component analysis (PCA). In addition, a new software package for the processing of GLORIA data is introduced which allows us to generate calibrated spectra from raw measurements in a semi-automated data processing chain.

The Arctic winter 2010/2011 was characterized by a persistent vortex with extremely low temperatures in the lower stratosphere above northern Scandinavia leading to a strong activation of chlorine compounds (ClOx) like Cl, Cl2, ClO, ClOOCl, OClO, and HOCl, which rapidly destroyed ozone when sunlight returned after winter solstice. The MIPAS-B (Michelson Interferometer for Passive Atmospheric Sounding) and TELIS (TErahertz and submillimeter LImb Sounder) balloon measurements obtained in northern Sweden on 31 March 2011 inside the polar vortex have provided vertical profiles of inorganic and organic chlorine species as well as diurnal variations of ClO around sunrise over the whole altitude range in which chlorine has been undergoing activation and deactivation. This flight was performed at the end of the winter during the last phase of ClOx deactivation. The complete inorganic and organic chlorine partitioning and budget for 31 March 2011, assumed to be representative for the late-winter Arctic stratosphere, has been derived by combining MIPAS-B and TELIS simultaneously observed molecules. A total chlorine amount of 3.41 ± 0.30 parts per billion by volume is inferred from the measurements (above 24 km). This value is in line with previous stratospheric observations carried out outside the tropics confirming the slightly decreasing chlorine amount in the stratosphere. Observations are compared and discussed with the output of a multi-year simulation performed with the chemistry climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry). The simulated stratospheric total chlorine amount is in accordance with the MIPAS-B/TELIS observations, taking into account the fact that some chlorine source gases and very short-lived species are not included in the model.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA), a Fourier-transform-spectrometer-based limb spectral imager, operates on high-altitude research aircraft to study the transit region between the troposphere and the stratosphere. It is one of the most sophisticated systems to be flown on research aircraft in Europe, requiring constant monitoring and human intervention in addition to an automation system. To ensure proper functionality and interoperability on multiple platforms, a flexible control and communication system was laid out. The architectures of the communication system as well as the protocols used are reviewed. The integration of this architecture in the automation process as well as the scientific campaign flight application context are discussed.

We report first chemistry mode retrieval results from the new airborne limb-imaging infrared FTS (Fourier transform spectrometer) GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) and comparisons with observations by the conventional airborne limb-scanning infrared FTS MIPAS-STR (Michelson Interferometer for Passive Atmospheric Sounding – STRatospheric aircraft). For GLORIA, the flights aboard the high-altitude research aircraft M55 Geophysica during the ESSenCe campaign (ESa Sounder Campaign 2011) were the very first in field deployment after several years of development. The simultaneous observations of GLORIA and MIPAS-STR during the flight on 16 December 2011 inside the polar vortex and under conditions of optically partially transparent polar stratospheric clouds (PSCs) provided us the first opportunity to compare the observations by two different infrared FTS generations directly. We validate the GLORIA results with MIPAS-STR based on the lower vertical resolution of MIPAS-STR and compare the vertical resolutions of the instruments derived from their averaging kernels. The retrieval results of temperature, HNO3, O3, H2O, CFC-11 and CFC-12 show reasonable agreement of GLORIA with MIPAS-STR and collocated in situ observations. For the horizontally binned hyperspectral limb images, the GLORIA sampling outnumbered the horizontal cross-track sampling of MIPAS-STR by up to 1 order of magnitude. Depending on the target parameter, typical vertical resolutions of 0.5 to 2.0 km were obtained for GLORIA and are typically a factor of 2 to 4 better compared to MIPAS-STR. While the improvement of the performance, characterization and data processing of GLORIA are the subject of ongoing work, the presented first results already demonstrate the considerable gain in sampling and vertical resolution achieved with GLORIA.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an airborne infrared limb imager combining a two-dimensional infrared detector with a Fourier transform spectrometer. It was operated aboard the new German Gulfstream G550 High Altitude LOng Range (HALO) research aircraft during the Transport And Composition in the upper Troposphere/lowermost Stratosphere (TACTS) and Earth System Model Validation (ESMVAL) campaigns in summer 2012. This paper describes the retrieval of temperature and trace gas (H2O, O3, HNO3) volume mixing ratios from GLORIA dynamics mode spectra that are spectrally sampled every 0.625 cm−1. A total of 26 integrated spectral windows are employed in a joint fit to retrieve seven targets using consecutively a fast and an accurate tabulated radiative transfer model. Typical diagnostic quantities are provided including effects of uncertainties in the calibration and horizontal resolution along the line of sight. Simultaneous in situ observations by the Basic Halo Measurement and Sensor System (BAHAMAS), the Fast In-situ Stratospheric Hygrometer (FISH), an ozone detector named Fairo, and the Atmospheric chemical Ionization Mass Spectrometer (AIMS) allow a validation of retrieved values for three flights in the upper troposphere/lowermost stratosphere region spanning polar and sub-tropical latitudes. A high correlation is achieved between the remote sensing and the in situ trace gas data, and discrepancies can to a large extent be attributed to differences in the probed air masses caused by different sampling characteristics of the instruments. This 1-D processing of GLORIA dynamics mode spectra provides the basis for future tomographic inversions from circular and linear flight paths to better understand selected dynamical processes of the upper troposphere and lowermost stratosphere.

The novel airborne Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) measures infrared emission of atmospheric trace constituents. GLORIA comprises a cooled imaging Fourier transform spectrometer, which is operated in unpressurized aircraft compartments at ambient temperature. The whole spectrometer is pointed by the gimbal towards the atmospheric target. In order to reach the required sensitivity for atmospheric emission measurements, the spectrometer optics needs to operate at a temperature below 220 K. A lightweight and compact design is mandatory due to limited space and high agility requirements. The cooled optical system needs to withstand high pressure and temperature gradients, humidity, and vibrations. A new cooling system based on carbon dioxide and liquid nitrogen combined with high-performance insulation has been developed to meet the mechanical, thermal, and logistical demands. The challenging mechanical and spatial requirements lead to the development of a novel rigid linear slide design in order to achieve the large optical path difference for high spectral resolution. This paper describes the mechanical and thermal setup of GLORIA and presents the performance results on two different research aircrafts.

The three-dimensional quantification of small-scale processes in the upper troposphere and lower stratosphere is one of the challenges of current atmospheric research and requires the development of new measurement strategies. This work presents the first results from the newly developed Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) obtained during the ESSenCe (ESa Sounder Campaign) and TACTS/ESMVal (TACTS: Transport and composition in the upper troposphere/lowermost stratosphere, ESMVal: Earth System Model Validation) aircraft campaigns. The focus of this work is on the so-called dynamics-mode data characterized by a medium-spectral and a very-high-spatial resolution. The retrieval strategy for the derivation of two- and three-dimensional constituent fields in the upper troposphere and lower stratosphere is presented. Uncertainties of the main retrieval targets (temperature, O3, HNO3, and CFC-12) and their spatial resolution are discussed. During ESSenCe, high-resolution two-dimensional cross-sections have been obtained. Comparisons to collocated remote-sensing and in situ data indicate a good agreement between the data sets. During TACTS/ESMVal, a tomographic flight pattern to sense an intrusion of stratospheric air deep into the troposphere was performed. It was possible to reconstruct this filament at an unprecedented spatial resolution of better than 500 m vertically and 20 × 20 km horizontally.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an imaging Fourier transform spectrometer that is capable of operating on various high-altitude research aircraft. It measures the atmospheric emission in the thermal infrared spectral region in limb and nadir geometry. GLORIA consists of a classical Michelson interferometer combined with an infrared camera. The infrared detector has a usable area of 128 × 128 pixels, measuring up to 16 384 interferograms simultaneously. Imaging Fourier transform spectrometers impose a number of challenges with respect to instrument calibration and algorithm development. The optical setup with extremely high optical throughput requires the development of new methods and algorithms for spectral and radiometric calibration. Due to the vast amount of data there is a high demand for scientifically intelligent optimisation of the data processing. This paper outlines the characterisation and processing steps required for the generation of radiometrically and spectrally calibrated spectra. Methods for performance optimisation of the processing algorithm are presented. The performance of the data processing and the quality of the calibrated spectra are demonstrated for measurements collected during the first deployments of GLORIA on aircraft.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an imaging limb emission sounder operating in the thermal infrared region. It is designed to provide measurements of the upper troposphere/lower stratosphere with high spatial and high spectral resolution. The instrument consists of an imaging Fourier transform spectrometer integrated into a gimbal. The assembly can be mounted in the belly pod of the German High Altitude and Long Range research aircraft (HALO) and in instrument bays of the Russian M55 Geophysica. Measurements are made in two distinct modes: the chemistry mode emphasises chemical analysis with high spectral resolution, and the dynamics mode focuses on dynamical processes of the atmosphere with very high spatial resolution. In addition, the instrument allows tomographic analyses of air volumes. The first measurement campaigns have shown compliance with key performance and operational requirements.

The upper troposphere/lower stratosphere (UTLS) represents an important part of the climate system. Even small changes in the composition and dynamic structure of this region have significant radiative effects. Quantifying the underlying physical and chemical processes therefore represents a crucial task. Currently, there is a lack of UTLS observations with sufficient three-dimensional resolution. The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) aircraft instrument addresses this observational lack by providing observations of numerous trace constituents as well as temperature and cloud structures with an unprecedented combination of vertical resolution (up to 300 m) and horizontal resolution (about 30 km &times 30 km). As a result, important scientific questions concerning stratosphere–troposphere exchange, the occurrence of subvisible cirrus clouds in the lowermost stratosphere (LMS), polar chemistry, and gravity wave processes can be addressed, as reviewed in this paper.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is a prototype of an imaging Fourier Transform Spectrometer (FTS) for PREMIER, a former candidate mission for ESA's Earth Explorer 7. GLORIA is deployed on board various research aircraft such as the Russian M55 Geophysica or the German HALO. The instrument provides detailed infrared images of the Upper Troposphere/Lower Stratosphere (UTLS) region, which plays a crucial role in the climate system. GLORIA uses a two-dimensional detector array for infrared limb observations in emission and therefore needs large-area blackbody radiation sources (126 mm × 126 mm) for calibration. In order to meet the highly demanding uncertainty requirements for the scientific objectives of the GLORIA missions and due to the sophisticated tomographic evaluation scheme, the spatial distribution of the radiance temperature of the blackbody calibration sources has to be determined with an uncertainty of about 0.1 K. Since GLORIA is exposed to the hostile environment of the UTLS with mutable low temperature and pressure, an in-flight calibration system has to be carefully designed to cope with those adverse circumstances. The GLORIA in-flight calibration system consists of two identical weight-optimised high-precision blackbody radiation sources, which are independently stabilised at two different temperatures. The two point calibration is in the range of the observed atmospheric infrared radiance emissions with 10 K below and 30 K above ambient temperature, respectively. Thermo-Electric Coolers are used to control the temperature of the blackbody radiation sources offering the advantage of avoiding cryogens and mechanical coolers. The design and performance of the GLORIA in-flight calibration system is presented. The blackbody calibration sources have been comprehensively characterised for their spatially (full aperture) and spectrally (7 to 13 μm) resolved radiation properties in terms of radiance temperatures traceable to the International Temperature Scale (ITS-90) at the Physikalisch-Technische Bundesanstalt (PTB), the national metrology institute of Germany.

The winter 2009/2010 was characterized by a strong Arctic vortex with extremely cold mid-winter temperatures in the lower stratosphere associated with an intense activation of reactive chlorine compounds (ClOx) from reservoir species. Stratospheric limb emission spectra were recorded during a flight of the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 24 January 2010 inside the Arctic vortex. Several fast limb sequences of spectra (in time steps of about 10 min) were measured from nighttime photochemical equilibrium to local noon allowing the retrieval of chlorine- and nitrogen-containing species which change rapidly their concentration around the terminator between night and day. Mixing ratios of species like ClO, NO2, and N2O5 show significant changes around sunrise, which are temporally delayed due to polar stratospheric clouds reducing the direct radiative flux from the sun. ClO variations were derived for the first time from MIPAS-B spectra. Daytime ClO values of up to 1.6 ppbv are visible in a broad chlorine activated layer below 26 km correlated with low values (below 0.1 ppbv) of the chlorine reservoir species ClONO2. Observations are compared and discussed with calculations performed with the 3-dimensional Chemistry Climate Model EMAC (ECHAM5/MESSy Atmospheric Chemistry). Mixing ratios of the species ClO, NO2, and N2O5 are well reproduced by the model during night and noon. However, the onset of ClO production and NO2 loss around the terminator in the model is not consistent with the measurements. The MIPAS-B observations along with Tropospheric Ultraviolet-Visible (TUV) radiation model calculations suggest that polar stratospheric clouds lead to a delayed start followed by a faster increase of the photodissoziation of ClOOCl and NO2 near the morning terminator since stratospheric clouds alter the direct and the diffuse flux of solar radiation. These effects are not considered in the EMAC model simulations which assume a cloudless atmosphere.

The first profile retrieval results of the Terahertz and submillimeter Limb Sounder (TELIS) balloon instrument are presented. The spectra are recorded during a 13-h balloon flight on 24 January 2010 from Kiruna, Sweden. The TELIS instrument was mounted on the MIPAS-B2 gondola and shared this platform with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and the mini-Differential Optical Absorption Spectroscopy (mini-DOAS) instruments. The flight took place within the Arctic vortex at an altitude of ≈34 km in chlorine activated air, and both active (ClO) and inactive chlorine (HCl) were measured over an altitude range of respectively ≈16–32 km and ≈10–32 km. In this altitude range, the increase of ClO concentration levels during sunrise has been recorded with a temporal resolution of one minute. During the daytime equilibrium, a maximum ClO level of 2.1 ± 0.3 ppbv has been observed at an altitude of 23.5 km. This equilibrium profile is validated against the ClO profile by the satellite instrument Microwave Limb Sounder (MLS) aboard EOS Aura. HCl profiles have been determined from two different isotopes – H35Cl and H37Cl – and are also validated against MLS. The precision of all profiles is well below 0.01 ppbv and the overall accuracy is therefore governed by systematic effects. The total uncertainty of these effects is estimated to be maximal 0.3 ppbv for ClO around its peak value at 23.5 km during the daytime equilibrium, and for HCl it ranges from 0.05 to 0.4 ppbv, depending on altitude. In both cases the main uncertainty stems from a largely unknown non-linear response in the detector.

GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) is a new remote sensing instrument essentially combining a Fourier transform infrared spectrometer with a two-dimensional (2-D) detector array in combination with a highly flexible gimbal mount. It will be housed in the belly pod of the German research aircraft HALO (High Altitude and Long Range Research Aircraft). It is unique in its combination of high spatial and state-of-the art spectral resolution. Furthermore, the horizontal view angle with respect to the aircraft flight direction can be varied from 45° to 135°. This allows for tomographic measurements of mesoscale events for a wide variety of atmospheric constituents. In this paper, a tomographic retrieval scheme is presented, which is able to fully exploit the manifold radiance observations of the GLORIA limb sounder. The algorithm is optimized for massive 3-D retrievals of several hundred thousands of measurements and atmospheric constituents on common hardware. The new scheme is used to explore the capabilities of GLORIA to sound the atmosphere in full 3-D with respect to the choice of the flightpath and to different measurement modes of the instrument using ozone as a test species. It is demonstrated that the achievable resolution should approach 200 m vertically and 20 km–30 km horizontally. Finally, a comparison of the 3-D inversion with conventional 1-D inversions using the assumption of a horizontally homogeneous atmosphere is performed.

Active chlorine species play a dominant role in the catalytic destruction of stratospheric ozone in the polar vortices during the late winter and early spring seasons. Recently, the correct understanding of the ClO dimer cycle was challenged by the release of new laboratory absorption cross sections (Pope et al., 2007) yielding significant model underestimates of observed ClO and ozone loss (von Hobe et al., 2007). Under this aspect, nocturnal Arctic stratospheric limb emission measurements carried out by the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) from Kiruna (Sweden) on 11 January 2001 and 20/21 March 2003 have been reanalyzed with regard to the chlorine reservoir species ClONO2 and the active species, ClO and ClOOCl (Cl2O2). New laboratory measurements of IR absorption cross sections of ClOOCl for various temperatures and pressures allowed for the first time the retrieval of ClOOCl mixing ratios from remote sensing measurements. High values of active chlorine (ClOx) of roughly 2.3 ppbv at 20 km were observed by MIPAS-B in the cold mid-winter Arctic vortex on 11 January 2001. While nighttime ClOOCl shows enhanced values of nearly 1.1 ppbv at 20 km, ClONO2 mixing ratios are less than 0.1 ppbv at this altitude. In contrast, high ClONO2 mixing ratios of nearly 2.4 ppbv at 20 km have been observed in the late winter Arctic vortex on 20 March 2003. No significant ClOx amounts are detectable on this date since most of the active chlorine has already recovered to its main reservoir species ClONO2. The observed values of ClOx and ClONO2 are in line with the established polar chlorine chemistry. The thermal equilibrium constants between the dimer formation and its dissociation, as derived from the balloon measurements, are on the lower side of reported data and in good agreement with values recommended by von Hobe et al. (2007). Calculations with the ECHAM/MESSy Atmospheric Chemistry model (EMAC) using established kinetics show similar chlorine activation and deactivation, compared to the measurements in January 2001 and March 2003, respectively.

Gravity wave (GW) remote sensing from space now has reached a stage of maturity that some first confinements for GW modeling can be deduced. This is in particular due to global distributions of absolute values of GW momentum flux from infrared limb sounders and due to 2-D maps of the horizontal wave field provided by nadir viewing instruments. The logical step forward is an infrared limb imager (ILI) which combines the good vertical resolution of limb sounding with horizontal mapping capabilities and provides 3-D images of the GW temperature structures. In this paper we investigate 1) how an ILI advances measurements of GW momentum flux, 2) which additional benefits are achieved by limb imaging of GWs, and 3) how an ILI compares to other GW momentum flux measurements, in-situ, ground-based, and from space. In particular, the large advance made by gaining regular 3-D sampling is demonstrated.

This paper presents the spatio-temporal distribution of NOy species at altitudes between 14 and 31 km as measured with the MIPAS-B instrument on the morning of 21 March 2003 in northern Scandinavia. At lower altitudes (below about 22 km), temperature variations, the distribution of ClONO2, and the tracer N2O reveal the dynamics through the edge of the late arctic polar vortex. At higher altitudes, continuous measurement before, during, and after sunrise provides information about photochemistry illustrating the evolution of the photochemically active gases NO2 and N2O5 around sunrise. The measured temporal evolution of NO2 and N2O5 is compared to box modelling that is run along backward calculated trajectories. While the comparison of measured and modelled N2O5 reveals significant differences, there is a good agreement between the model and observations for NO2 in terms of volume mixing ratios but the simulated decrease shortly after sunrise is underestimated compared to the measurements. The differences are attributed to the photolysis rates used in the box model calculations.

The Improved Limb Atmospheric Spectrometer (ILAS)-II sensor aboard the Japanese ADEOS-II satellite was launched into its sun-synchronous orbit on 14 December 2002 and performed solar occultation measurements of trace species, aerosols, temperature, and pressure in the polar stratosphere until 25 October 2003. Vertical trace gas profiles obtained with the balloon version of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-B) provide one of the sparse data sets for validating ILAS-II version 2 and 1.4 data. The MIPAS-B limb emission spectra were collected on 20 March 2003 over Kiruna (Sweden, 68° N) at virtually the same location that has been sounded by ILAS-II about 5.5 h prior to the sampling of MIPAS-B. The intercomparison of the new ILAS-II version 2 (Northern Hemispheric sunrise) data to MIPAS-B vertical trace gas profiles shows a good to excellent agreement within the combined error limits for the species O3, N2O, CH4, H2O (above 21 km), HNO3, ClONO2, and CFC-11 (CCl3F) in the compared altitude range between 16 and 31 km such that these data appear to be very useful for scientific analysis. With regard to the previous version 1.4 ILAS-II data, significant improvements in the consistency with MIPAS-B are obvious especially for the species CH4 and H2O, but also for O3, HNO3, ClONO2, NO2, and N2O5. However, comparing gases like NO2, N2O5, and CFC-12 (CCl2F2) exhibits only poor agreement with MIPAS-B such that these species cannot be assumed to be validated at the present time.

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) has been operating since March 2002 onboard of the ENVIronmental SATellite of the European Space Agency (ESA). The high resolution (0.035 cm−1 full width half maximum, unapodized) limb-emission measurements acquired by MIPAS in the first two years of operation have very good geographical and temporal coverage and have been re-processed by ESA with the most recent versions (4.61 and 4.62) of the inversion algorithms. The products of this processing chain are pressures at the tangent points and geolocated profiles of temperature and of the volume mixing ratios of six key atmospheric constituents: H2O, O3, HNO3, CH4, N2O and NO2. As for all the measurements made with innovative instruments and techniques, this data set requires a thorough validation. In this paper we present a geophysical validation of the temperature profiles derived from MIPAS measurements by the ESA retrieval algorithm. The validation is carried-out by comparing MIPAS temperature with correlative measurements made by radiosondes, lidars, in-situ and remote sensors operated either from the ground or stratospheric balloons. The results of the intercomparison indicate that the bias of the MIPAS profiles is generally smaller than 1 or 2 K depending on altitude. Furthermore we find that, especially at the edges of the altitude range covered by the MIPAS scan, the random error estimated from the intercomparison is larger (typically by a factor of two to three) than the corresponding estimate derived on the basis of error propagation. In this work we also characterize the discrepancies between MIPAS temperature and the temperature fields resulting from the analyses of the European Centre for Medium-range Weather Forecasts (ECMWF). The bias and the standard deviation of these discrepancies are consistent with those obtained when comparing MIPAS to correlative measurements; however, in this case the detected bias has a peculiar behavior as a function of altitude. This behavior is very similar to that observed in previous studies and is suspected to be due to vertical oscillations in the ECMWF temperature. The current understanding is that, at least in the upper stratosphere (above ≈10 hPa), these oscillations are caused by a discrepancy between model biases and biases of assimilated radiances from primarily nadir sounders.

Altitude profiles of ClONO2 retrieved with the IMK (Institut für Meteorologie und Klimaforschung) science-oriented data processor from MIPAS/Envisat (Michelson Interferometer for Passive Atmospheric Sounding on Envisat) mid-infrared limb emission measurements between July 2002 and March 2004 have been validated by comparison with balloon-borne (Mark IV, FIRS2, MIPAS-B), airborne (MIPAS-STR), ground-based (Spitsbergen, Thule, Kiruna, Harestua, Jungfraujoch, Izaña, Wollongong, Lauder), and spaceborne (ACE-FTS) observations. With few exceptions we found very good agreement between these instruments and MIPAS with no evidence for any bias in most cases and altitude regions. For balloon-borne measurements typical absolute mean differences are below 0.05 ppbv over the whole altitude range from 10 to 39 km. In case of ACE-FTS observations mean differences are below 0.03 ppbv for observations below 26 km. Above this altitude the comparison with ACE-FTS is affected by the photochemically induced diurnal variation of ClONO2. Correction for this by use of a chemical transport model led to an overcompensation of the photochemical effect by up to 0.1 ppbv at altitudes of 30–35 km in case of MIPAS-ACE-FTS comparisons while for the balloon-borne observations no such inconsistency has been detected. The comparison of MIPAS derived total column amounts with ground-based observations revealed no significant bias in the MIPAS data. Mean differences between MIPAS and FTIR column abundances are 0.11±0.12×1014 cm−2 (1.0±1.1%) and −0.09±0.19×1014 cm−2 (−0.8±1.7%), depending on the coincidence criterion applied. χ2 tests have been performed to assess the combined precision estimates of MIPAS and the related instruments. When no exact coincidences were available as in case of MIPAS – FTIR or MIPAS – ACE-FTS comparisons it has been necessary to take into consideration a coincidence error term to account for χ2 deviations. From the resulting χ2 profiles there is no evidence for a systematic over/underestimation of the MIPAS random error analysis.