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In this paper, we present the updated SAGE-CCI-OMPS+ climate data record of monthly zonal mean ozone profiles. This dataset covers the stratosphere and combines measurements by nine limb and occultation satellite instruments – SAGE II (Stratospheric Aerosol and Gases Experiment II), OSIRIS (Optical Spectrograph and InfraRed Imaging System), MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), SCIAMACHY (SCanning Imaging Spectrometer for Atmospheric CHartographY), GOMOS (Global Ozone Monitoring by Occultation of Stars), ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer), OMPS-LP (Ozone Monitor Profiling Suite Limb Profiler), POAM (Polar Ozone and Aerosol Measurement) III, and SAGE III/ISS (Stratospheric Aerosol and Gases Experiment III on the International Space Station). Compared to the original version of the SAGE-CCI-OMPS dataset (Sofieva et al., 2017b), the update includes new versions of MIPAS, ACE-FTS, and OSIRIS datasets and introduces data from additional sensors (POAM III and SAGE III/ISS) and retrieval processors (OMPS-LP). In this paper, we show detailed intercomparisons of ozone profiles from different instruments and data versions, with a focus on the detection of possible drifts in the datasets. The SAGE-CCI-OMPS+ dataset has a better coverage of polar regions and of the upper troposphere and the lower stratosphere (UTLS) than the previous dataset. We also studied the influence of including new datasets on ozone trends, which are estimated using multiple linear regression. The changes in the merged dataset do not change the overall morphology of post-1997 ozone trends; statistically significant trends are observed in the upper stratosphere. The largest changes in ozone trends are observed in polar regions, especially in the Southern Hemisphere. The updated SAGE-CCI-OMPS+ dataset contains profiles of deseasonalized anomalies and ozone concentrations from 1984 to 2021, in 10∘ latitude bins from 90∘ S to 90∘ N and in the altitude range from 10 to 50 km. The dataset is open access and available at https://climate.esa.int/en/projects/ozone/data/ (last access: 9 March 2023) and at ftp://cci_web@ftp-ae.oma.be/esacci (ESA Climate Office; last access: 9 March 2023).

Trends in stratospheric trace gases like HCl, N2O, O3, and NOy show a hemispheric asymmetry over the last two decades, with trends having opposing signs in the Northern and Southern Hemispheres. Here we use N2O, a long-lived tracer with a tropospheric source, as a proxy for stratospheric circulation in the multiple linear regression model used to calculate stratospheric trace gas trends. This is done in an effort to isolate trends due to circulation changes from trends due to ozone depleting substances. We use measurements from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) and the Optical Spectrograph and InfraRed Imager System (OSIRIS), and model results from the Whole Atmosphere Community Climate Model (WACCM). Trends in HCl, O3, and NOy for 2004–2018 are examined. Using the N2O regression proxy, we show that observed HCl increases in the Northern Hemisphere are due to changes in the stratospheric circulation. We also show that negative O3 trends above 30 hPa in the Northern Hemisphere can be explained by change in the circulation, but that negative ozone trends at lower levels cannot. Trends in stratospheric NOy are found to be largely consistent with trends in N2O.

Air quality measurements from geostationary orbit by the upcoming instrument TEMPO (Tropospheric Emissions: Monitoring of Pollution) will offer an unprecedented view of atmospheric composition over North America. Measurements over Canadian latitudes, however, offer unique challenges: TEMPO's lines of sight are shallower, the sun is lower, and snow cover is more common. All of these factors increase the impact of the sphericity and the horizontal inhomogeneity of the atmosphere on the accuracy of the air quality measurements. Air mass factors encapsulate the complex paths of the measured sunlight, but traditionally they ignore horizontal variability. For the high spatial resolution of modern instruments such as TEMPO, the error due to neglecting horizontal variability is magnified and needs to be characterized. Here we present developments to SASKTRAN, the radiative transfer framework developed at the University of Saskatchewan, to calculate air mass factors in a spherical atmosphere, with and without consideration of horizontal inhomogeneity. Recent upgrades to SASKTRAN include first order spherical corrections for the discrete ordinates method and the capacity to compute air mass factors with the Monte Carlo method. Together with finite difference air mass factors via the successive orders method, this creates a robust framework for computing air mass factors. One dimensional air mass factors from all three methods are compared in detail and are found to be in good agreement. Two-dimensional air mass factors are computed with the deterministic successive orders method, demonstrating an alternative for a calculation which would typically be done only with a non-deterministic Monte Carlo method. The two-dimensional air mass factors are used to analyze a simulated scene with TEMPO over the Canadian oil sands. The effect of a sharp horizontal feature in surface albedo and surface NO2 was quantified while varying the distance of the feature from the intended measurement location. Such a feature in the surface albedo or surface NO2 could induce errors on the order of 5 to 10 % at a distance of 50 km, and their combination could induce errors on the order of 10 % as far as 100 km away.

The 2022 eruption of the Hunga Tonga-Hunga Ha’apai volcano caused substantial impacts on the atmosphere, including a large increase of stratospheric aerosol at high altitudes and a massive injection of water vapor. We show results from application of a two-dimensional tomographic retrieval of aerosol extinction profiles from limb scattered sunlight made by the NASA OMPS Limb Profiler instrument. The tomographic retrieval substantially improves the agreement in magnitude and vertical structure with coincident lidar and occultation observations compared to the standard retrieval. We also show a secondary effect of bias from uncertainty in assumed particle size distribution parameters that results in a systematic underestimation of the aerosol extinction in the altitude region of the peak of the volcanic aerosol layer.

For the past 17 years, the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) instrument on the Canadian SCISAT satellite has been measuring profiles of atmospheric ozone. The latest operational versions of the level 2 ozone data are versions 3.6 and 4.1. This study characterizes how both products compare with correlative data from other limb-sounding satellite instruments, namely MAESTRO, MLS, OSIRIS, SABER, and SMR. In general, v3.6, with respect to the other instruments, exhibits a smaller bias (which is on the order of ∼ 3 %) in the middle stratosphere than v4.1 (∼ 2 %–9 %); however, the bias exhibited in the v4.1 data tends to be more stable, i.e. not changing significantly over time in any altitude region. In the lower stratosphere, v3.6 has a positive bias of about 3 %–5 % that is stable to within ±1 % per decade, and v4.1 has a bias on the order of −1 % to +5 % and is also stable to within ±1 % per decade. In the middle stratosphere, v3.6 has a positive bias of ∼ 3 % with a significant negative drift on the order of 0.5 %–2.5 % per decade, and v4.1 has a positive bias of 2 %–9 % that is stable to within ±0.5 % per decade. In the upper stratosphere, v3.6 has a positive bias that increases with altitude up to ∼ 16 % and a significant negative drift on the order of 2 %–3 % per decade, and v4.1 has a positive bias that increases with altitude up to ∼ 15 % and is stable to within ±1 % per decade. Estimates indicate that both versions 3.6 and 4.1 have precision values on the order of 0.1–0.2 ppmv below 20 km and above 45 km (∼ 5 %–10 %, depending on altitude). Between 20 and 45 km, the estimated v3.6 precision of ∼ 4 %–6 % is better than the estimated v4.1 precision of ∼ 6 %–10 %.

We develop an algorithm that uses the aerosol extinction at two wavelengths (color ratio) to derive the size and number density for stratospheric aerosols. We apply our algorithm to Ozone Mapping Profiler Suite Limb Profiler (OMPS-LP) L2 and Stratospheric Aerosol and Gas Experiment (SAGE) data. We show that the color ratio between two wavelengths (e.g. 510 nm/869 nm) is insensitive to aerosol concentration and thus can be used to derive aerosol size assuming a log-normal size distribution. With the size and the extinction, we can compute a number density consistent with both wavelengths. Our results compare favorably to balloon borne particle size and concentration measurements. Our results are also consistent with SAGE solar occultation measurements. Finally, we show the background distribution of stratospheric aerosols and the changes in those distributions during the Reikoke and Hunga Tonga-Hunga Ha’apai volcanic eruptions. We also show the evolution of the size and number density of aerosols following both of those eruptions.

The Limb Imaging Fourier-Transform Spectrometer Experiment (LIFE) instrument is a balloon-borne prototype of a satellite instrument designed to take vertical images of atmospheric limb emission spectra in the 700 to 1400 cm−1 wavenumber range from the upper troposphere/lower stratosphere (UTLS) altitude region of the atmosphere. The prototype builds on the success of past and existing instruments while reducing the complexity of the imaging design. This paper details the results of a demonstration flight on a stabilized stratospheric balloon gondola from Timmins, Canada in August 2019. Retrievals of vertical trace gas profiles for the important greenhouse gases H2O, O3, CH4 and N2O, as well as HNO3, are performed using an Optimal Estimation Approach and the SASKTRAN radiative transfer model. The retrieved profiles are compared to approximately coincident observations made by the ACE-FTS solar occultation satellite instrument. An evaluation of the LIFE measurements is performed and areas of improvement are identified. This work increases the overall technical readiness of the approach for future balloon, aircraft and space applications.

In this paper, we present the updated SAGE-CCI-OMPS+ climate data record of monthly zonal mean ozone profiles. This dataset covers the stratosphere and combines measurements by 9 limb and occultation satellite instruments – SAGE II, OSIRIS, MIPAS, SCIAMACHY, GOMOS, ACE-FTS, OMPS-LP, POAM III and SAGE III/ISS. Compared to the original version of the SAGE-CCI-OMPS dataset (Sofieva et al., 2017), the update includes new versions of MIPAS, ACE-FTS, and OSIRIS datasets, and introduces data from additional sensors (POAM III, SAGE III/ISS) and retrieval processors (OMPS-LP). In the paper, we show detailed intercomparisons of ozone profiles from different instruments and data versions, with a focus on the detection of possible drifts in the datasets. The SAGE-CCI-OMPS+ dataset has a better coverage of polar regions and of the upper troposphere and the lower stratosphere (UTLS) than the SAGE-CCI-OMPS dataset. We also studied the influence of including new datasets on ozone trends, which are estimated using multiple linear regression. The changes in the merged dataset do not change the overall morphology of post-1997 ozone trends: statistically significant trends are observed in the upper stratosphere. The largest changes in ozone trends are observed in polar regions, especially in the Southern Hemisphere. The updated SAGE-CCI-OMPS+ dataset contains profiles of deseasonalized anomalies and ozone concentrations from 1984 to 2021, in 10° latitude bins from 90° S to 90° N, and in the altitude range from 10 km to 50 km. The dataset is in open access at https://climate.esa.int/en/projects/ozone/data/ and at ftp://cci_web@ftp-ae.oma.be/esacci (ESA Climate Office, last access: 10 August 2022).

The v7.2 NO2 retrieval for the Optical Spectrograph and InfraRed Imager System (OSIRIS) was designed to improve sensitivity in the upper troposphere–lower stratosphere (UTLS) and to reduce an observed low bias in the previous version, v6.0. The details of this retrieval are described and then the data are compared to coincident NO2 profiles from the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE-FTS) and the Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS). The PRATMO photochemical box model was used to account for differences in the measurement times of the instruments: all datasets were scaled to the same local solar time of 12:00 LST. Coincident ACE-FTS and OSIRIS NO2 measurements agree within 20 % throughout much of the stratosphere. Coincident SAGE III/ISS and OSIRIS NO2 measurements also agree within 20 %, with OSIRIS biased low at all altitudes and latitudes. The ACE-FTS, OSIRIS, and SAGE III-ISS NO2 monthly zonal mean data show very similar variability in time at most altitude and latitudes.

A comprehensive inter-comparison of seven radiative transfer models in the limb scattering geometry has been performed. Every model is capable of accounting for polarization within a spherical atmosphere. Three models (GSLS, SASKTRAN-HR, and SCIATRAN) are deterministic, and four models (MYSTIC, SASKTRAN-MC, Siro, and SMART-G) are statistical using the Monte Carlo technique. A wide variety of test cases encompassing different atmospheric conditions, solar geometries, wavelengths, tangent altitudes, and Lambertian surface reflectances have been defined and executed for every model. For the majority of conditions it was found that the models agree to better than 0.2 % in the single-scatter test cases and better than 1 % in the scalar and vectorial test cases with multiple scattering included, with some larger differences noted at high values of surface reflectance. For the first time in limb geometry, the effect of atmospheric refraction was compared among four models that support it (GSLS, SASKTRAN-HR, SCIATRAN, and SMART-G). Differences among most models with multiple scattering and refraction enabled were less than 1 %, with larger differences observed for some models. Overall the agreement among the models with and without refraction is better than has been previously reported in both scalar and vectorial modes.

The v7.2 NO2 retrieval for the Optical Spectrograph and InfraRed Imager System (OSIRIS) was designed to improve sensitivity in the Upper Troposphere-Lower Stratosphere (UTLS) and to reduce an observed low bias in the previous version, v6.0. The details of this retrieval are described, and then the data are compared to coincident NO2 profiles from the Atmospheric Chemistry Experiment – Fourier Transform Spectrometer (ACE-FTS) and the Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS). The the PRATMO photochemical box model was used to account for differences in the measurement times of the instruments: all datasets were scaled to the same local solar time of 12:00 pm. Coincident ACE-FTS and OSIRIS NO2 measurements agree within 20 % throughout much of the stratosphere. Coincident SAGE III/ISS and OSIRIS NO2 measurements also agree within 20 %, with OSIRIS biased low at all altitudes and latitudes. The ACE-FTS, OSIRIS, and SAGE III-ISS NO2 monthly zonal mean data show very similar variability in time at most altitude and latitudes.

Deep convection within the Asian summer monsoon (ASM) transports surface level air into the upper troposphere-lower stratosphere (UTLS). This work aims to understand the distribution of NO

The Stratospheric Aerosol and Gas Experiment (SAGE) III has been operating on the International Space Station (ISS) since mid-2017. Nitrogen dioxide (NO2) number density profiles are routinely retrieved from SAGE III/ISS solar occultation measurements in the middle atmosphere. Although NO2 density varies throughout the day due to photochemistry, the standard SAGE NO2 retrieval algorithm neglects these variations along the instrument's line of sight by assuming that the number density has a constant gradient within a given vertical layer of the atmosphere. This assumption will result in a retrieval bias for a species like NO2 that changes rapidly across the terminator. In this work we account for diurnal variations in retrievals of NO2 from the SAGE III/ISS measurements, and we determine the impact of this algorithm improvement on the resulting NO2 number densities. The first step in applying the diurnal correction is to use publicly available SAGE III/ISS products to convert the retrieved number density profiles to optical depth profiles. The retrieval is then re-performed with a new matrix that applies photochemical scale factors for each point along the line of sight according to the changing solar zenith angle. In general NO2 that is retrieved by accounting for these diurnal variations is more than 10 % lower than the standard algorithm below 30 km. This effect is greatest in winter at high latitudes and generally greater for sunrise occultations than sunset. Comparisons with coincident profiles from the Optical Spectrograph and InfraRed Imager System (OSIRIS) show that NO2 from SAGE III/ISS is generally biased high; however the agreement improves by up to 20 % in the mid-stratosphere when diurnal variations are accounted for in the retrieval. We conclude that diurnal variations along the SAGE III/ISS line of sight are an important term to consider for NO2 analyses at altitudes below 30 km.

Improving knowledge of the ozone global distributions in the mesosphere–lower thermosphere (MLT) is a crucial step in understanding the behaviour of the middle atmosphere. However, the concentration of ozone under sunlit conditions in the MLT is often so low that its measurement requires instruments with very high sensitivity. Fortunately, the bright oxygen airglow can serve as a proxy to retrieve the daytime ozone density indirectly, due to the strong connection to ozone photolysis in the Hartley band. The OSIRIS IR imager (hereafter, IRI), one of the instruments on the Odin satellite, routinely measures the oxygen infrared atmospheric band (IRA band) at 1.27 µm. In this paper, we will primarily focus on the detailed description of the steps done for retrieving the calibrated IRA band limb radiance (with

After decades of depletion in the 20th century, near-global ozone now shows clear signs of recovery in the upper stratosphere. The ozone column, however, remained largely constant since the turn of the century, mainly due to changes in the lower stratosphere. In the tropical lower stratosphere, ozone is expected to decrease as a consequence of enhanced upwelling driven by increasing greenhouse gas concentrations, and this is consistent with observations. There is recent evidence, however, that mid-latitude ozone continues to decrease as well, contrary to model predictions. These changes are likely related to dynamical variability, but the impact of changing circulation patterns on stratospheric ozone is not well understood. Here we use merged measurements from the Stratospheric Aerosol and Gas Experiment II (SAGE II), the Optical Spectrograph and InfraRed Imaging System (OSIRIS), and SAGE III/ISS to quantify ozone changes in the 2000–2021 period. We implement a sampling correction for the OSIRIS and SAGE III/ISS datasets, and assess trend significance taking into account temporal differences with respect to Aura Microwave Limb Sounder data. We show that ozone increased by 2–6 % in the upper and 1–3 % in the middle stratosphere since 2000, while lower stratospheric ozone decreased by similar amounts. These decreases are significant in the tropics (>95 % confidence), but not necessarily at mid-latitudes (> 80 % confidence). In the upper and middle stratosphere, changes since 2010 point to hemispheric asymmetries in ozone recovery. Significant positive trends are present in the southern hemisphere, while ozone at northern mid-latitudes has remained largely unchanged in the last decade. These differences might be related to asymmetries and long-term variability in the Brewer-Dobson circulation. Circulation changes impact ozone in the lower stratosphere as well. In tropopause relative coordinates, most of the negative trends in the tropics lose significance, highlighting the impacts of a warming tropopause and increasing tropopause altitudes.

Die Mesopausenregion in einer Höhe von 80-100 km ist ein Bereich der Atmosphäre, der schwer zu erforschen ist, da direkte Messungen kaum möglich sind. Eine Möglichkeit bieten aber Messungen des Airglows. Airglow entsteht, wenn elektromagnetische Strahlung durch chemische Reaktionen ausgesendet wird. Diese kann dann mit Satelliten oder vom Boden aus gemessen werden. Eine Reaktion bei der Airglow entsteht ist die Reaktion von Natrium mit Ozon. Bei dieser Reaktion, die auch Chapman-Mechanismus genannt wird, entsteht angeregtes Natrium mit zwei unterschiedlichen Gesamtdrehimpulsquantenzahlen. Die Abregung in den Grundzustand führt dann zu den zwei bekannten Natrium D-Linien (D2=589,0 nm; D1=589,6 nm). Wie hoch der Anteil des Natriums, der durch die Reaktion in den angeregten Zustand übergeht ist, ist dabei noch nicht genau geklärt. Das Verhältnis von Natrium im Grundzustand und Natrium im angeregten Zustand wird durch die branching ratio f beschrieben. Deren Wert wird in der aktuellen Forschung zwischen 5 und 16 % geschätzt. In dieser Arbeit soll, durch Vergleich verschiedener Messungen von unabhängigen Instrumenten, dieser Wert weiter eingegrenzt werden. Im Zentrum stehen dabei die Messungen des Instrumentes OSIRIS auf dem Satelliten ODIN und der Vergleich zu Messungen, die mit verschiedenen bodengestützten Natrium-Lidars gemacht worden sind. Das Ergebnis ist eine Schätzung der branching ratio auf ca. 6 %.

Sodium airglow is generated when excited sodium atoms emit electromagnetic radiation while they are relaxing from an excited state into a lower energetic state. This electromagnetic radiation, the two sodium D lines at 589.0 and 589.6 nm, can usually be detected from space or from ground. Sodium nightglow occurs at times when the sun is not present and excitation of sodium atoms is a result of chemical reaction with ozone. The detection of sodium nightglow can be a means to determine the amount of sodium in the earth's mesosphere and lower thermosphere (MLT). In this study, we present time series of monthly mean sodium concentration profiles, by utilizing the large spatial and temporal coverage of satellite sodium D-line nightglow measurements. We use the OSIRIS/Odin mesospheric limb measurements to derive sodium concentration profiles and vertical column densities and compare those to measurements from SCIAMACHY/Envisat and GOMOS/Envisat. Here we show that the Na D-line limb emission rate (LER) and volume emission rate (VER) profiles calculated from the OSIRIS and SCIAMACHY measurements, although the OSIRIS LER and VER profiles are around 25 % lower, agree very well in shape and overall seasonal variation. The sodium concentration profiles also agree in shape and magnitude, although those do not show the clear semi-annual cycle which is present in the LER and VER profiles. The comparison to the GOMOS sodium vertical column densities (VCDs) shows that the OSIRIS VCDs are of the same order of magnitude although again the semi-annual cycle is not as clear. We attribute the differences in the LER, VER and sodium profiles to the differences in spatial coverage between the OSIRIS and SCIAMACHY measurements, the lower signal-to-noise ratio (SNR) of the SCIAMACHY measurements and differences in local time between the measurements of the two satellites.

Decreases in stratospheric NOx associated with enhanced aerosol have been observed after large volcanic eruptions, for example, after the eruption of Mount Pinatubo in 1991. While the 1991 Mount Pinatubo eruption was the last large explosive eruption, recent studies have shed light on the impacts of moderate-sized eruptions since the year 2000 on the global stratospheric aerosol budget. We use an ensemble of simulations from a coupled climate-chemistry model to quantify and analyze changes in NO and NO2 (NOx), N2O5, HNO3, ClO, and ClONO2 during periods of increased stratospheric volcanic aerosol concentrations since 2000. By using an ensemble approach, we are able to distinguish forced responses from internal variability. We also compare the model ensemble results to satellite measurements of these changes in atmospheric composition, including measurements from the Optical Spectrograph and Infrared Imaging Spectrometer on the Odin satellite and the Aura Microwave Limb Sounder. We find decreases in stratospheric NOx concentrations up to 20 hPa, consistent with increases in stratospheric HNO3 concentrations. The HNO3 perturbations also extend higher, up to 5 hPa, associated with periods of increased volcanic aerosol concentrations in both model simulations and observations, though correlations with volcanic aerosol are considerably higher in the model simulations. The model simulates increases in ClO at altitudes and magnitudes similar to the NOx reductions, but this response is below the detectable limit in the available observations (100 pptv). We also demonstrate the value of accounting for transport-related anomalies of atmospheric trace gases by regression onto N2O anomalies.

Stratospheric aerosols are of a great importance to the scientific community, predominantly because of their role in climate, but also because accurate knowledge of aerosol characteristics is relevant for trace gas retrievals from remote-sensing instruments. There are several data sets published which provide aerosol extinction coefficients in the stratosphere. However, for the instruments measuring in the limb-viewing geometry, the use of this parameter is associated with uncertainties resulting from the need to assume an aerosol particle size distribution (PSD) within the retrieval process. These uncertainties can be mitigated if PSD information is retrieved. While occultation instruments provide more accurate information on the aerosol extinction coefficient, in this study, it was shown that limb instruments are more sensitive to the smaller particles in the visible–near-infrared spectral range. However, the sensitivity of occultation instruments improves if the UV part of the wavelength spectrum is considered. A data set containing PSD information was recently retrieved from SCIAMACHY limb measurements and provides two parameters of the unimodal lognormal PSD for the SCIAMACHY operational period (2002–2012). In this study, the data set is expanded by aerosol extinction coefficients and Ångström exponents calculated from the retrieved PSD parameters. Parameter errors for the recalculated Ångström exponents and aerosol extinction coefficients are assessed using synthetic retrievals. For the extinction coefficient the resulting parameter error is within ±25 %, and for the Ångström exponent, it is better than 10 %. The SCIAMACHY aerosol extinction coefficients recalculated from PSD parameters are compared to those from SAGE II. The differences between the instruments vary from 0 % to 25 % depending on the wavelength. Ångström exponent comparison with SAGE II shows differences between 10 % at 31 km and 40 % at 18 km. Comparisons with SAGE II, however, suffer from the low number of collocated profiles. Furthermore, the Ångström exponents obtained from the limb-viewing instrument OSIRIS are used for the comparison. This comparison shows an average difference within 7 %. The time series of these differences do not show signatures of any remarkable events (e.g., volcanic eruptions or biomass burning events). In addition, the temporal behaviour of the Ångström exponent in the tropics is analyzed using the SCIAMACHY data set. It is shown that there is no trivial relation between the Ångström exponent value at a single wavelength pair and the PSD because the same value of Ångström exponent can be obtained from an infinite number of combinations of the PSD parameters.

The OH airglow has been used to investigate the chemistry and dynamics of the mesosphere and the lower thermosphere (MLT) for a long time. The infrared imager (IRI) aboard the Odin satellite has been recording the night-time 1.53 µm OH (3-1) emission for more than 15 years (2001–2015), and we have recently processed the complete data set. The newly derived data products contain the volume emission rate profiles and the Gaussian-approximated layer height, thickness, peak intensity and zenith intensity, and their corresponding error estimates. In this study, we describe the retrieval steps for these data products. We also provide data screening recommendations. The monthly zonal averages depict the well-known annual oscillation and semi-annual oscillation signatures, which demonstrate the fidelity of the data set (https://doi.org/10.5281/zenodo.4746506, Li et al., 2021). The uniqueness of this Odin IRI OH long-term data set makes it valuable for studying various topics, for instance, the sudden stratospheric warming events in the polar regions and solar cycle influences on the MLT.

Wildfire-driven pyro-convection (PyroCb) is capable of lofting combustion products into the stratosphere, polluting it with smoke aerosols at hemispheric and yearly scales. This realization has emerged after the record-breaking British Columbia PyroCb event in August 2017 that approached moderate volcanic eruptions in terms of stratospheric aerosol load perturbation. The Australian “Black Summer” bushfires in 2019/20 have surpassed the previous record by a factor of 3 and rivaled the strongest volcanic eruptions in the XXI century. Here we exploit a synergy of various satellite observations, ECMWF meteorological analysis and radiative transfer modeling to quantify the perturbation of stratospheric particulate and gaseous composition, dynamical circulation and radiative balance caused by the Australian New Year’s PyroCb outbreak. One of the most striking repercussions of this event was the generation of several persistent anticyclonic vortices that provided confinement to the PyroCb plumes and preserved them from rapid dilution in the environment. The most intense vortex measured 1000 km in diameter, persisted in the stratosphere for over 13 weeks and lifted a confined bubble of combustion gases, aerosols and moisture to 35 km altitude. It was accompanied by a synoptic-scale ozone hole with the total column reduction by about 30%. The startling consequences of the Australian event provide new insights into climate-altering potential of the wildfires, that have increased in frequency and strength over the recent years.

The Aerosol Limb Imager (ALI) is a multi-spectral imager capable designed to observe aerosol extinction and particle size profiles in the upper-troposphere lower-stratosphere. ALI uses a system of linear polarizers, a liquid crystal rotator, and an acoustic-optic tunable filter to select the linear polarization state and wavelength of limb scattered sunlight radiance between 600 nm and 1500 nm. From stratospheric balloon, spectral images have spatial resolution of

The eruption of Raikoke on June 22nd, 2019 was one of the largest in recent decades, spewing approximately 1.5 Tg of sulfur up to 17 km altitude. This eruption has been widely studied using a combination of climate models and measurement systems, including ground based lidars, in situ particle counters, and a variety of satellite platforms. The early plume has been well categorized by high-resolution measurements from CALIPSO, MODIS, VIIRS, IASI and other nadir viewing instruments, but as the plume ages investigation often shifts to limb sounding instruments that provide greater sensitivity to lower aerosol levels. These instruments have proven critical in understanding the long-term radiative and climatic impacts of stratospheric aerosol burdens after these explosive events, but the complexity of the measurements, sampling, and retrievals has made error characterization in high-loading conditions difficult.This work explores systematic biases in limb measurements after the Raikoke eruption due to a variety of factors often implicit in the retrievals and analysis. Near-coincident CALIPSO, SAGE III and OMPS-LP measurements are used to investigate saturation of limb-sounding measurement in the early plume. The recent OMPS-LP v2 stratospheric aerosol product is compared with the University of Saskatchewan product to investigate benefits and drawbacks of the tomographic approach. SAGE III measurements are used as a validation when available although coverage limitations preclude comparisons in the thickest parts of the plume. This work highlights the subtleties in comparing limb observations, with implications for model comparisons after large events such as volcanic eruptions and forest fires. Not only in the early plume, where sampling can be sparse, but also in the weeks and months following the eruption.

Smoke from wildfires are a significant source of air pollution, which can adversely impact ecosystems and the air quality in downwind populated areas. With increasing severity of wildfires over the years, these are a significant threat to air quality in densely populated areas. Emissions from wildfires are most commonly estimated by a bottom-up approach, using proxies such fuel type, burn area, and emission factors. Emissions are also commonly derived with a top-down approach, using satellite observed Fire Radiative Power. Furthermore, wildfire emissions can also be estimated directly from satellite-borne measurements.Here, we present advancements and improvements of direct emission estimates of forest fire NOx emissions by using TROPOMI (Tropospheric Monitoring Instrument) high-resolution satellite datasets, including NO2 vertical column densities (VCDs) and information on plume height and aerosol scattering. The effect of smoke aerosols on the sensitivity of TROPOMI to NO2 (via air mass factors) is estimated with recalculated VCDs, and validated with aircraft observations. Different top-down emission estimation methods are tested on synthetic data to determine the accuracy, and the sensitivity to parameters, such as wind fields, satellite sampling, instrument noise, NO2:NOx conversion ratio, species atmosphere lifetime and plume spread. Lastly, the top-down, bottom-up and direct emission estimates of fire emissions are quantitatively compared.

Using a combination of different measurement techniques is important to understand the numerous processes happening in the MLT-region. One of those processes is the excitation of atomic sodium by reaction with ozone which leads to emission of electromagnetic radiation: a phenomenon called Airglow. Although the sodium excitation mechanism was already proposed in 1939 by Sidney Chapman and further investigation was done by a great number of scientists, there are still some key parameters that are not well-known today. One of those parameters is the branching ratio fA which determines the amount of sodium in the excited state. Exact knowledge of this value would offer the opportunity to use Na-nightglow measurements to determine sodium profiles in the MLT-region. In this study we used both, satellite measurements and ground-based Lidar measurements to help approach a more reliable branching ratio fA. By comparing measurements that were made by the two instruments OSIRIS on Odin (Satellite) and the Lidar of the Colorado State University (ground-based) we found a branching ratio fA of 0.064 +- 0.028.

The Spatial Heterodyne Observations of Water instrument (SHOW) is a limb imaging instrument that is being developed to provide accurate, dense, high vertical resolution measurements of water vapour in the upper troposphere and lower stratosphere. SHOW utilizes a field widened spatial heterodyne spectrometer operating in the limb viewing configuration to observe limb scattered sunlight in a small ~3 nm spectral window centered near 1365 nm. Vertically resolved images of the limb absorption spectrum are obtained with each frame that are inverted using non-linear optimal estimation to extract the vertical distribution of water vapour. The large throughput and high spectral resolution (0.02 nm unapodized) provided by the field widened SHS allows vertical profiles with a target vertical resolution of < 500 m to be obtained with rapid along track sampling (~50 km below 20 km and between 100 km – 300 km above 20 km) from a low earth orbit satellite. In this paper, we present the SHOW measurement concept and examine the practical considerations that influence design tradeoffs. We discuss the challenges and solutions that have been identified to optimize the instrument configuration and present an end-to-end simulation of the level 0 measurements, calibrations and level 2 water vapour product.

The Stratospheric Aerosol and Gas Experiment (SAGE) III has been operating on the International Space Station (ISS) since mid 2017. Nitrogen dioxide (NO2) number density profiles are routinely retrieved from SAGE III/ISS solar occultation measurements in the middle atmosphere. Although NO2 density varies throughout the day due to photochemistry, the standard SAGE NO2 retrieval algorithm neglects these variations along the instrument's line of sight by assuming that the number density has a constant gradient within a given vertical layer of the atmosphere. This assumption will result in a retrieval bias for a species like NO2 that changes rapidly across the terminator. In this work we account for diurnal variations in retrievals of NO2 from the SAGE III/ISS measurements, and determine the impact of this algorithm improvement on the resulting NO2 number densities. The diurnal correction is applied by first undoing the SAGE III/ISS retrieval using publicly available SAGE III/ISS products to obtain an optical depth profile. The retrieval is then performed with a new matrix that applies photochemical scale factors for each point along the line of sight according to the changing solar zenith angle. In general NO2 that is retrieved by accounting for these diurnal variations is more than 10 % lower than the standard algorithm below 30 km. This effect is greatest in winter at high latitudes, and generally greater for sunrise occultations than sunset. Comparisons with coincident profiles from the Optical Spectrograph and InfraRed Imager System (OSIRIS) show that NO2 from SAGE III/ISS is generally biased high, however the agreement improves by up to 20 % in the mid stratosphere when diurnal variations are accounted for in the retrieval. We conclude that diurnal variations along the SAGE III/ISS line of sight are an important term to consider for NO2 analyses at altitudes below 30 km.

A robust stratospheric aerosol climate data record enables the depiction of the radiative forcing of this highly variable component of climate. Since stratospheric aerosol also plays a key role in the chemical processes leading to ozone depletion, stratosphere is one of the crucial parameters in understanding climate change in the past and potential changes in the future. As a part of Stratospheric-tropospheric Processes and their Role in Climate (SPARC) Stratospheric Sulfur and its Role in Climate (SSiRC) activity, the Global Space-based Stratospheric Aerosol Climatology (GloSSAC) was created (Thomason et al., 2018) to support the World Climate Research Programme (WCRP)’s Coupled Model Intercomparison Project Phase 6 (CMIP6) (Zanchettin et al., 2016). This data set is a follow-on to one created as a part of Stratosphere-Troposphere Process and their Role in Climate Project (SPARC)’s Assessment of Stratospheric Aerosol Properties (ASAP) activity(SPARC, 2006) and a data created for Chemistry-Climate Model Initiative (CCMI) in 2012 (Eyring and Lamarque, 2012). Herein, we discuss changes to the original release version including those as a part of v1.1 that was released in September 2018 that primarily corrects an error in the conversion of Cryogenic Limb Array Etalon Spectrometer (CLAES) data to Stratospheric Aerosol and Gas Experiment (SAGE) II wavelengths, and the new release, v2.0. Version 2.0 is focused on improving the post-SAGE II era (after 2005) with the goal to mitigate elevated aerosol extinction in the lower stratosphere at mid and high latitudes noted in v1.0 as noted in Thomason et al. (2018). Changes include the use of version 7.0 of Optical Spectrograph and InfraRed Imaging System(OSIRIS), the recently released Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) Lidar Level 3 Stratospheric Aerosol profile monthly product, and the new addition of SAGE III/ISS. Although, the version 7.0 OSIRIS data is substantially improved at its native wavelength of 750 nm, conversion to 525 nm using a constant Angstrom exponent often results in disagreements with SAGEII/ SAGE III/ISS overlap measurements. We, therefore use an observed relationship between OSIRIS extinction at 750 nm and SAGEII/SAGE III/ISS extinction at 525 nm to derive Altitude-Latitude based monthly climatology of Angstrom exponent to compute extinction at 525 nm, resulting in a better agreement between OSIRIS and SAGE measurements. We employ a similar approach to convert OSIRIS 750 nm extinction to 1020 nm extinction for the post-SAGEII period. Additionally, we incorporate the recently released standard CALIPSO stratospheric aerosol profile monthly product into GloSSAC with an improved conversion technique of 532 nm backscatter coefficient to extinction using an observed relationship between OSIRIS 525 nm extinction and CALIPSO 532 nm backscatter. We also investigate for any cloud contamination in OSIRIS/standard CALIPSO stratospheric aerosol product, which may have caused apparent enhancement in the aerosol extinction particularly in the lower stratosphere. SAGE III/ISS data is also incorporated in GloSSAC to extend the climatology to the present and to test the approach used to correct OSIRIS/CALIPSO data. The GloSSAC v2.0 netcdf file is accessible at https://doi.org/10.5067/glossac-l3-v2.0 (Thomason, 2020).

We report on the measurement of the transmittance and reflectance of unpolarized light (425–700 nm) in three birefringent, acousto-optic materials, including quartz, lithium niobate, and tellurium dioxide, after exposure to varying fluences of proton radiation ( 10 14 − 10 18 p r o t o n s / c m 2 ) delivered by a 10 keV hydrogen ion beamline. We observe a general monotonic decrease in transmittance with increasing fluence for all three materials, but with varying rates of change and critical points of change. Reflectance measurements also exhibit a general monotonic trend with fluence, but increases in quartz are observed versus decreases in both lithium niobate and tellurium dioxide. These observations are used to assess the suitability of the materials for acousto-optic applications in the space environment where charged particles from the solar wind are dominant and pose a threat to device operation. Our measurements agree with previously reported work concluding that tellurium dioxide is suitable for space applications at low fluences (below 10 16 i o n s / c m 2 ), but our findings also raise previously unreported concerns for higher accumulated fluences observed for longer mission lifetimes of greater than five to 10 years in space in an unshielded configuration.

The Spatial Heterodyne Observations of Water instrument (SHOW) is a limb-sounding satellite prototype that utilizes the Spatial Heterodyne Spectroscopy (SHS) technique, operating in a limb-viewing configuration, to observe limb-scattered sunlight in a vibrational band of water vapour within a spectral window from 1363 to 1366 nm. The goal is to retrieve high vertical and horizontal resolution measurements of water vapour in the upper troposphere and lower stratosphere. The prototype instrument has been configured for observations from NASA's ER-2 high-altitude airborne remote science airplane. Flying at a maximum altitude of ∼21.34 km with a maximum speed of ∼760 km h−1, the ER-2 provides a stable platform to simulate observations from a low-earth orbit satellite. Demonstration flights were performed from the ER-2 during an observation campaign from 15 to 22 July 2017. In this paper, we present the laboratory characterization work and the level 0 to level 1 processing of flight data that were obtained during an engineering flight performed on 18 July 2017. Water vapour profile retrievals are presented and compared to in situ radiosonde measurements made of the same approximate column of air. These measurements are used to validate the SHOW measurement concept and examine the sensitivity of the technique.

TROPOMI, on-board the Sentinel-5 Precursor satellite is a nadir-viewing spectrometer measuring reflected sunlight in the ultraviolet, visible, near-infrared, and shortwave infrared spectral range. From these spectra several important air quality and climate-related atmospheric constituents are retrieved at an unprecedented high spatial resolution, including nitrogen dioxide (NO(2)). We present the first retrievals of TROPOMI NO(2) over the Canadian Oil Sands, contrasting them with observations from the OMI satellite instrument, and demonstrate its ability to resolve individual plumes and highlight its potential for deriving emissions from individual mining facilities. Further, the first TROPOMI NO(2) validation is presented, consisting of aircraft and surface in-situ NO(2) observations, as well as ground-based remote-sensing measurements between March and May 2018. Our comparisons show that the TROPOMI NO(2) vertical column densities are highly correlated with the aircraft and surface in-situ NO(2) observations, and the ground-based remote-sensing measurements with a low bias (15–30 %) over the Canadian Oil Sands. PLAIN LANGUAGE SUMMARY: Nitrogen dioxide (NO(2)) is a pollutant that is linked to respiratory health issues and has negative environmental impacts such as soil and water acidification. Near the surface the most significant sources of NO(2) are fossil fuel combustion and biomass burning. With a recently launched satellite instrument (TROPOspheric Monitoring Instrument; TROPOMI) NO(2) can be measured with an unprecedented combination of accuracy, spatial coverage, and resolution. This work presents the first TROPOMI NO(2) measurements near the Canadian Oil Sands and shows that these measurements have an outstanding ability to detect NO(2) on a very high horizontal resolution that is unprecedented for satellite NO(2) observations. Further, these satellite measurements are in excellent agreement with aircraft and ground-based measurements.

During the last 2 years (2018-2019) a series of volcanic eruptions led to remarkable enhancements in stratospheric aerosol load. These are eruptions of Ambae (July 2018, Vanuatu), Raikoke (June 2019, Russia) and Ulawun (July 2019, Papua New Guinea). In this study we examine the evolution of the stratospheric aerosol bulk optical properties following these events in consideration of large-scale stratospheric circulation. We use long-term aerosol records by ground-based lidars in both hemispheres together with global observations by various satellite missions (OMPS-LP, SAGE III, OSIRIS, CALIOP) and discuss the consistency between these datasets. In addition, we evaluate the preliminary lower stratosphere aerosol product by ESA Aeolus mission through intercomparison with ground-based lidars. The 28-yr Observatoire de Haute Provence (OHP) lidar record shows that Raikoke eruption has led to the strongest enhancement of stratospheric aerosol optical depth (SAOD) in the northern extratropics since Pinatubo eruption. Satellite observations suggest that the stratospheric plume of Raikoke has dispersed throughout the entire Northern hemisphere and ascended up to 27 km altitude. The eruption of Ulawun in the tropics has further boosted the stratospheric aerosol load and by Fall 2019, the global mean SAOD was a factor of 2.5 higher than its background level. At the turn of the year 2020, while both Raikoke and Ulawun aerosols were still present in the stratosphere, a dramatic bushfire event accompanied by vigorous fire-induced thunderstorms (PyroCb) in eastern Australia caused a massive injection of smoke into the stratosphere. The early detections of stratospheric smoke by OMPS-LP suggest that the zonal-mean SAOD perturbation caused by this event exceeds the previous record-breaking PyroCb-related perturbation after the British Columbia fires in August 2017. We use satellite observations of aerosol and trace gases (H2O, CO) to characterize the stratospheric impact of the wildfires and contrast it with that of volcanic eruptions.

Limb scatter instruments in the UV-Vis spectral range have provided longterm global records of stratospheric aerosol extinction important for climate records and modelling. While comparisons with occultation instruments show generally good agreement, the source and magnitude of the biases arising from retrieval assumptions, approximations in the radiative transfer modelling, and inversion techniques has not been thoroughly characterized. This paper explores the biases between SCIAMACHY v1.4, OSIRIS v5.07 and SAGE II v7.00 aerosol extinctions through a series of coincident comparisons as well as simulation and retrieval studies to investigate the cause and magnitude of the various systematic differences. The effect of a priori profiles, particle size assumptions, radiative transfer modelling, inversion techniques, and the different satellite datasets are explored. It is found that the assumed a priori profile can have a large effect near the normalization point, as well as systematic influence at lower altitudes. The error due to particle size assumptions is relatively small when averaged over a range of scattering angles, but individual errors depend on the particular scattering angle, particle size and measurement vector definition. Differences due to radiative transfer modelling introduce differences between the retrieved products of less than 10 % on average, but can introduce vertical structure. The combination of the different scenario simulations and the application of both algorithms to both datasets enable the origin of some of the systematic features such as high altitude differences when compared to SAGE II to be explained.