Abstract. Three-dimensional measurements of gravity waves are required in order to quantify their directionresolved momentum fluxes and obtain a better understanding of their propagation characteristics. Such 3-D measurements of gravity waves in the lowermost stratosphere have been provided by the airborne Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) using full angle tomography. Closed flight patterns of sufficient size are needed to acquire the full set of angular measurements for full angle tomography. These take about 2 h and are not feasible everywhere due to scientific reasons or air traffic control restrictions. Hence, this paper investigates the usability of limited angle tomography for gravity wave research based on synthetic observations. Limited angle tomography uses only a limited set of angles for tomographic reconstruction and can be applied to linear flight patterns. A synthetic end-toend simulation has been performed to investigate the sensitivity of limited angle tomography to gravity waves with different wavelengths and orientations with respect to the flight path. For waves with wavefronts roughly perpendicular to the flight path, limited angle tomography and full angle tomography can derive wave parameters like wavelength, amplitude, and wave orientation with similar accuracy. For waves with a horizontal wavelength above 200 km and vertical wavelength above 3 km, the wavelengths can be retrieved with less than 10 % error, the amplitude with less than 20 % error, and the horizontal wave direction with an error below 10 • . This is confirmed by a comparison of results obtained from full angle tomography and limited angle tomography for real measurements taken on 25 January 2016 over Iceland. The reproduction quality of gravity wave parameters with limited angle tomography, however, depends strongly on the orientation of the waves with respect to the flight path. Thus, full angle tomography might be preferable in cases in which the orientation of the wave cannot be predicted or waves with different orientations exist in the same volume and thus the flight path cannot be adjusted accordingly. Also, for low-amplitude waves and short-scale waves full angle tomography has advantages due to its slightly higher resolution and accuracy.

Abstract. 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.

Abstract. During winter 2015/2016 the Arctic stratosphere was characterized by extraordinarily low temperatures in connection with the occurrence of extensive polar stratospheric clouds. From mid of December 2015 until mid of March 2016 the German research aircraft HALO (High Altitude and Long–Range Research Aircraft) was deployed to probe the lowermost stratosphere in the Arctic region within the POLSTRACC (Polar Stratosphere in a Changing Climate) mission. More than twenty flights have been conducted out of Kiruna/Sweden and Oberpfaffenhofen/Germany, covering the whole winter period. Besides total reactive nitrogen (NOy), observations of nitrous oxide, nitric acid, ozone and water were used for this study. Total reactive nitrogen and its partitioning between gas- and particle phase are key parameters for understanding processes controlling the ozone budget in the polar winter stratosphere. The redistribution of total reactive nitrogen was evaluated by using tracer–tracer correlations. In January air masses with extensive nitrification were encountered at altitudes between 12 and 15 km. The excess NOy amounted up to about 6 ppb. During several flights, along with gas–phase nitrification, indications for extensive occurrence of nitric acid containing particles at flight altitude were found. These observations support the assumption of sedimentation and subsequent evaporation of nitric acid containing particles leading to redistribution of total reactive nitrogen. Remnants of nitrified air masses have been observed until mid of March. Between end of February and mid of March also de-nitrified air masses have been observed in connection with high potential temperatures. Using tracer–tracer correlations, missing total reactive nitrogen was estimated to amount up to 6 ppb. This indicates the downward transport of air masses that have been denitrified during the earlier winter phase. Observations within POLSTRACC, at the bottom of the vortex, reflect heterogeneous processes from the overlying Arctic winter stratosphere. The comparison of the observations with CLaMS model simulations confirm and complete the picture arising from the present measurements. The simulations confirm, that the ensemble of all observations is representative for the vortex–wide vertical NOy-redistribution.

Abstract. 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 of PAN, 1400 pptv for C2H6, 800 pptv for HCOOH, 4500 pptv for CH3OH, and 200 pptv for C2H4. One flight shows 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 are likely originating from 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 simulation 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, too. However, C2H6 and HCOOH are generally underestimated by the model, while CH3OH and C2H4, the species with the shortest atmospheric lifetimes of the discussed pollution trace gases, 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.

Abstract. Multiple limb sounder measurements of the same atmospheric region taken from different directions can be combined in a 3D tomographic retrieval. Mathematically, this is a computationally expensive inverse modelling problem. It typically requires an introduction of some general knowledge of the atmosphere (regularisation) due to its underdetermined nature. This paper introduces a consistent, physically motivated (no ad-hoc unphysical parameters) variant of the Tikhonov regularisation scheme based on spatial derivatives of first and second order. As shown by a case study with synthetic data, this scheme, 5 combined with irregular grid retrieval methods, improves both upon the quality and the computational cost of 3D tomography, while eliminating grid dependence and the need to tune parameters for each use case. The few physical parameters required can be derived from in situ measurements and model data. An efficient Monte Carlo technique was adopted for retrieval accuracy estimation.