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Ammonia (NH 3) 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. NH 3 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 NH 3 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 NH 3 of more than 1 ppbv in the Asian monsoon upper troposphere but no clear indication of NH 3 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 NH 3 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, NH 3 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 NH 3 during transport to the upper troposphere may be underestimated for the biomass burning cases above the South Atlantic. Since NH 3 is strongly undersampled, in particular at higher altitudes, we hope for regular vertically resolved measurements of NH 3 from the proposed CAIRT (Changing-Atmosphere Infra-Red Tomography Explorer) mission to strengthen our understanding of this important trace gas in the atmosphere. [ABSTRACT FROM AUTHOR]

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 has been operated onboard the research aircraft Geophysica within the Asian Monsoon during the StratoClim campaign (July 2017) and onboard HALO (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. 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 reproduce the biomass burning plumes above the South Atlantic in general. However, NH3 concentrations are largely overestimated by the CAMS models within these plumes. We suggest that emission strengths used by CAMS models are of different accuracy for biomass burning and 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 mission to strengthen our understanding of this important trace gas in the atmosphere. [ABSTRACT FROM AUTHOR]

MIPAS-B2 is a balloon-borne limb-emission sounder for atmospheric research. The heart of the instrument is a Fourier spectrometer that covers the mid-infrared spectral range (4-14 [micro]m) and operates at cryogenic temperatures. Essential for this application is the sophisticated line-of-sight stabilization system, which is based on an inertial navigation system and is supplemented with an additional star reference system. The major scientific benefit of the instrument is the simultaneous detection of complete trace gas families in the stratosphere without restrictions concerning the time of day and viewing directions. The specifications, the design considerations, the actual realization of the instrument, and the results of characterization measurements that have been performed are described. OCIS codes: 120.6200, 010.1280.

The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an infrared imaging FTS spectrometer with a 2-D infrared detector operated on two high flying research aircrafts. It has flown on eight campaigns and measured along more than 300 000km of flight track. This paper details our instrument calibration and characterization efforts, which in particular leverage almost exclusively in-flight data. First, we present the framework of our new calibration scheme, which uses information from all three available calibration measurements (two blackbodies and upward pointing "deep space" measurements). Part of this scheme is a new correction algorithm correcting the erratically changing non-linearity of a subset of detector pixels and the identification of remaining bad pixels. Using this new calibration, we derive a 1-σ bound of 1% on the instrumental gain error and a bound of 30nWcm-2sr-1cm on the instrumental 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 derive a pointing accuracy of 0.032°, which corresponds to one detector pixel. The paper concludes with a brief study on how these newly characterised instrumental parameters affect temperature and ozone retrievals.We find that, first, the pointing uncertainty and, second, the instrumental gain uncertainty introduce the largest error in the result. [ABSTRACT FROM AUTHOR]

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 (VMR) 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. Since PAN has the longest lifetime of this foursome, elevated quantities of this molecule could be measured even in the lowermost stratosphere (locally up to 14 km). Backward trajectory calculations as well as global three-dimensional 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 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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The first stratospheric measurements of the diurnal variation of 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 parts per trillion by volume (pptv) were detected in the 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), 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 mid-latitudes from Timmins (49°N, Canada) in September 2014. Mean BrONO2 mixing ratios of 22pptv were observed after sunset in the altitude region between 21 and 29km. 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 of BrONO2 is in principal agreement with the balloon-borne observations. Using the nighttime simulated ratio between BrONO2 and Bry, the amount of Bry observed by MIPAS-B was estimated to about 21-25pptv in the lower stratosphere. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

We analyze polar stratospheric cloud (PSC) signatures in airborne MIPAS-STR (Michelson Interferometer for Passive Atmospheric Sounding - STRatospheric aircraft) observations in the spectral regions from 725 to 990 and 1150 to 1350 cm-1 under conditions suitable for the existence of nitric acid trihydrate (NAT) above northern Scandinavia on 11 December 2011. The high-resolution infrared limb emission spectra of MIPAS-STR show a characteristic "shoulder-like" signature in the spectral region around 820 cm-1, which is attributed to the ν2 symmetric deformation mode of NO-3 in β-NAT. Using radiative transfer calculations involving Mie and T-Matrix methods, the spectral signatures of spherical and aspherical particles are simulated. The simulations are constrained using collocated in situ particle measurements. Simulations assuming highly aspherical spheroids with aspect ratios (AR) of 0.1 or 10.0 and a lognormal particle mode with a mode radius of 4.8 μm reproduce the observed spectra to a high degree. A smaller lognormal mode with a mode radius of 2.0 μm, which is also taken into account, plays only a minor role. Within the scenarios analyzed, the best overall agreement is found for elongated spheroids with AR=0.1. Simulations of spherical particles and spheroids with AR=0.5 and 2.0 return results very similar to each other and do not allow us to reproduce the signature around 820 cm-1. The observed "shoulder-like" signature is explained by the combination of the absorption/ emission and scattering characteristics of large highly aspherical β-NAT particles. The size distribution supported by our results corresponds to ~9 ppbv of gas-phase equivalent HNO3 at the flight altitude of ~18.5 km. The results are compared with the size distributions derived from the in situ observations, a corresponding Chemical Lagrangian Model of the Stratosphere (CLaMS) simulation, and excess gas-phase HNO3 observed in a nitrification layer directly below the observed PSC. The presented results suggest that large highly aspherical β-NAT particles involved in denitrification of the polar stratosphere can be identified by means of passive infrared limb emission measurements. [ABSTRACT FROM AUTHOR]

We analyse polar stratospheric cloud (PSC) signatures in airborne MIPAS-STR (Michelson Interferometer for Passive Atmospheric Sounding - STRatospheric aircraft) observations under conditions suitable for the existence of nitric acid trihydrate (NAT) above northern Scandinavia on 11 December 2011. The high resolution infrared limb emission spectra of MIPAS-STR show a characteristic "shoulder-like" signature in the spectral region around 820 cm-1, which is attributed to the ν2 deformation mode of NO3- in β-NAT. Using radiative transfer calculations involving Mie and T-Matrix methods, the spectral signatures of spherical and aspherical particles are simulated. The simulations are constrained using collocated in-situ particle measurements. Simulations assuming highly aspherical spheroids with aspect ratios (AR) of 0.1 or 10.0 and a lognormal particle mode with a mode radius of 4.8 μm reproduce the observed spectra to a high degree. A smaller lognormal mode with a mode radius of 2.0 μm, which was also taken into account, plays only a minor role. Best overall agreement is found for elongated spheroids with AR = 0.1. Simulations of spherical particles and spheroids with AR = 0.5 and 2.0 return results very similar to each other and do not allow to reproduce the signature around 820 cm-1. The observed "shoulder-like" signature is explained by the combination of the emission and scattering characteristics of large highly aspherical β-NAT particles. The size distribution supported by our results corresponds with ~9 ppbv of gas-phase equivalent HNO3 at the flight altitude of ~18.5 km. The results are compared with the size distributions derived from the in-situ observations, a corresponding Chemical Lagrangian Model of the Stratosphere (CLaMS) simulation, and excess gas-phase HNO3 observed in a nitrification layer directly below the observed PSC. The presented results suggest that large highly aspherical β-NAT particles involved in denitrification of the polar stratosphere can be identified by means of passive infrared limb emission measurements. [ABSTRACT FROM AUTHOR]