Technical note: Lowermost-stratosphere moist bias in ECMWF IFS model diagnosed from airborne GLORIA observations during winter–spring 2016

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

Retrieval of Water Vapour Profiles from GLORIA Nadir Observations

We present the first analysis of water vapour profiles derived from nadir measurements by the infrared imaging Fourier transform spectrometer GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere). The measurements were performed on 27 September 2017, during the WISE (Wave driven ISentropic Exchange) campaign aboard the HALO aircraft over the North Atlantic in an area between 37°–50°N and 20°–28°W. From each nadir recording of the 2-D imaging spectrometer, the spectral radiances of all non-cloudy pixels have been averaged after application of a newly developed cloud filter. From these mid-infrared nadir spectra, vertical profiles of H2O have been retrieved with a vertical resolution corresponding to five degrees of freedom below the aircraft. Uncertainties in radiometric calibration, temperature and spectroscopy have been identified as dominating error sources. Comparing retrievals resulting from two different a priori assumptions (constant exponential vs. ERA 5 reanalysis data) revealed parts of the flight where the observations clearly show inconsistencies with the ERA 5 water vapour fields. Further, a water vapour inversion at around 6 km altitude could be identified in the nadir retrievals and confirmed by a nearby radiosonde ascent. An intercomparison of multiple water vapour profiles from GLORIA in nadir and limb observational modes, IASI (Infrared Atmospheric Sounding Interferometer) satellite data from two different retrieval processors, and radiosonde measurements shows a broad consistency between the profiles. The comparison shows how fine vertical structures are represented by nadir sounders as well as the influence of a priori information on the retrievals

Biomass burning pollution in the South Atlantic upper troposphere: GLORIA trace gas observations and evaluation of the CAMS model

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

Long-term validation of MIPAS ESA operational products using MIPAS-B measurements

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

Pollution trace gas distributions and their transport in the Asian monsoon upper troposphere and lowermost stratosphere during the StratoClim campaign 2017

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 (C$_2$H$_2$), 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 C$_2$H$_2$, and more than 200\,pptv of HCOOH are observed. Air masses with increased volume mixing ratios of PAN and C$_2$H$_2$ 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 (NH$_3$), 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 (NO$_2$) 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

Technical note: lowermost-stratospheric moist bias in ECMWF IFS model diagnosed from airborne GLORIA observations during winter/spring 2016

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 vapour measurements by the airborne infrared limb-imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) during the PGS (POLSTRACC/GW-LCYLCE-II/SALSA) campaign to study the LMS moist bias in ECMWF analyses and 12 h forecasts in the season from January to March 2016. Thereby, we exploit the 2-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 peaking at +50 % at potential vorticity levels of 6 to 10 PVU. In the diagnosed time period, the moist bias reduces at the highest and driest air masses observed, but clearly persists at lower levels until mid-March. Sensitivity experiments with more frequent temporal output, lower horizontal resolution, and higher/lower vertical resolution, show the short-term forecasts to be practically insensitive to these parameters on time scales of < 12 hours. Our results confirm that the diagnosed moist bias is present already in the initial conditions (i.e., the analysis) and thus supports the hypothesis that the cold bias develops as a result of forecast initialisation. The moist bias in the analysis might be explained by a model bias and/or the lack of water vapour observations suitable for assimilation by the model above the tropopause

Diurnal variations of BrONO₂ observed by MIPAS-B at midlatitudes and in the Arctic

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

Challenge of modelling GLORIA observations of upper troposphere-lowermost stratosphere trace gas and cloud distributions at high latitudes: A case study with state-of-The-Art models

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 (H$_{2}$O), ozone (O$_{3}$), nitric acid (HNO$_{3}$) 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 O$_{3}$, EMAC H$_{2}$O and EMAC HNO$_{3}$ distributions. Finally, we use sensitivity simulations to investigate (i) short-term cirrus cloud impacts on the H$_{2}$O distribution (ICON-ART), (ii) the overall impact of polar winter chemistry and microphysical processing on O$_{3}$ and HNO$_{3}$ (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 HNO$_{3}$. 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

Unusual chlorine partitioning in the 2015/16 Arctic winter lowermost stratosphere: Observations and simulations

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 (\chem{O_3}) and chlorine nitrate (\chem{ClONO_2}), 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. \chem{ClONO_2} volume mixing ratios up to 1100\,pptv were measured at 380\,K potential temperature in mesoscale structures. Similar mesoscale structures are also visible in \chem{O_3} 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 \chem{ClONO_2} 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 \chem{ClONO_2}, 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 \chem{O_3} and reactive nitrogen (\chem{NO_\mathit{y}}) due to ozone depletion and sedimentation of \chem{NO_\mathit{y}}-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 \chem{ClONO_2} measured by GLORIA. In February, most of the enhanced \chem{ClONO_2} 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 \chem{ClONO_2} have been transported in the remnants of the polar vortex towards the location of measurement for at least~11\,d