Michelson Interferometer For Passive Atmospheric Sounding Research Articles

IMK–IAA MIPAS retrieval version 8: CH4 and N2O

Abstract. Using the IMK–IAA data processor, methane and nitrous oxide distributions were retrieved from version-8 limb emission spectra recorded with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). The dataset includes measurements from the nominal, upper troposphere–lower stratosphere, middle-atmosphere, upper-atmosphere and noctilucent-cloud observation modes. The processing differs from the previous version-5 data with respect to the atmospheric state variables that are jointly retrieved along with the target gases CH4 and N2O, the treatment of the radiance offset, the selection of microwindows, the regularization, the spectroscopic data used and the treatment of horizontal variability of the atmospheric state. Besides the regular data product, a coarse-grid representation of the profiles with unity averaging kernels is available, as well as a specific research product for middle-atmosphere measurements resulting from a slightly different retrieval approach. The CH4 errors are dominated by the large spectroscopic uncertainty for line intensities, which probably is too pessimistic, and estimated to be 21 %–34 % in the altitude range 6–68 km for northern midlatitude summer day conditions. The N2O errors are 7 %–17 % below 45 km. At higher altitudes they increase strongly due to nearly vanishing N2O amounts. Analysis of the horizontal averaging kernels reveals that for both gases the horizontal resolution is sampling-limited; i.e., information is not smeared over consecutive limb scans. Zonal-mean seasonal composites of both CH4 and N2O exhibit the typical distribution of source gases with strong upwelling in the tropics and subsidence above the winter poles. Comparison with the previous data version shows several improvements: first, the vertical resolution of the retrieved CH4 (N2O) profiles has generally been significantly enhanced and varies between 2.5 (2.5) and 4 (5) km at altitudes between 10 and 60 km, with the best resolution around 30 km for both species. Secondly, the number of non-converged retrievals has been clearly reduced, and thirdly, formerly strongly oscillating profiles are now considerably smoother.

Version 8 IMK/IAA MIPAS measurements of CFC-11, CFC-12, and HCFC-22

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat provided infrared limb emission spectra, which were used to infer global distributions of CFC-11, CFC-12, and HCFC-22. Spectra were analysed using constrained non-linear least-squares fitting. Changes with respect to earlier data versions refer to the use of version 8 spectra, the altitude range where the background continuum is considered, details of the regularization and microwindow selection, and the occasional joint fitting of interfering species, the use of new spectroscopic data, the joint fit of a tangent-height-dependent spectral offset, and the use of 2D temperature fields. In the lower stratosphere the error budget is dominated by uncertainties in spectroscopic data, while above this measurement noise is the leading error source. The vertical resolution of CFC-11 and CFC-12 is 2–3 km near the tropopause, about 4 km at 30 km altitude, and 6–10 km at 50 km. The vertical resolution of HCFC-22 is somewhat coarser, 3–4 km at the tropopause and 10–12 km at 35 km altitude. In the altitude range of interest, the horizontal resolution is typically limited by the horizontal sampling of the measurements, not by the smearing of the retrievals. Horizontal information displacement does not exceed 150 km, which can become an issue only for comparisons with model simulations with high horizontal resolution or localized in situ observations. Along with the regular data product, an alternative representation of the data on a coarser vertical grid is offered. These data can be used without consideration of the averaging kernels. The new data version provides improvement with respect to reduction of biases and improved consistency between the full- and reduced-resolution mission period of MIPAS.

MIPAS ozone retrieval version 8: middle-atmosphere measurements

Abstract. We present a new version of O3 data retrieved from the three Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observation modes that we refer to for simplicity as the modes of the middle atmosphere (middle atmosphere, MA; upper atmosphere, UA; and noctilucent cloud, NLC). The O3 profiles cover altitudes from 20 up to 100 km for the daytime and up to 105 km at nighttime, for all latitudes, and the period 2005 until 2012. The data have been obtained with the IMK–IAA (Institute of Meteorology and Climate Research and Instituto de Astrofísica de Andalucía) MIPAS level-2 data processor and are based on ESA version-8 re-calibrated radiance spectra with improved temporal stability. The processing included several improvements with respect to the previous version, such as the consistency of the microwindows and spectroscopic data with those used in the nominal-mode V8R data, the O3 a priori profiles, and updates of the non-local thermodynamic equilibrium (non-LTE) parameters and the nighttime atomic oxygen. In particular, the collisional relaxation of O3(v1,v3) by the atomic oxygen was reduced by a factor of 2 in order to obtain a better agreement of nighttime mesospheric O3 with “non-LTE-free” measurements. Random errors are dominated by the measurement noise with 1σ values for single profiles for the daytime of < 5 % below ∼ 60 km, 5 %–10 % between 60 and 70 km, 10 %–20 % at 70–90 km, and about 30 % at 95 km. For nighttime, they are very similar below 70 km but smaller above (10 %–20 % at 75–95 km, 20 %–30 % at 95–100 km and larger than 30 % above 100 km). The systematic error is ∼ 6 % below ∼ 60 km (dominated by uncertainties in spectroscopic data) and 8 %–12 % above ∼ 60 km, mainly caused by non-LTE uncertainties. The systematic errors in the 80–100 km range are significantly smaller than in the previous version. The major differences with respect to the previous version are as follows: (1) the new retrievals provide O3 abundances in the 20–50 km altitude range that are larger by about 2 %–5 % (0.2–0.5 ppmv); (2) O3 abundances were reduced by ∼ 2 %–4 % between 50 and 60 km in the tropics and mid-latitudes; (3) O3 abundances in the nighttime O3 minimum just below 80 km were reduced, leading to a more realistic diurnal variation; (4) daytime O3 concentrations in the secondary maximum at the tropical and middle latitudes (∼ 40 %, 0.2–0.3 ppmv) were larger; and (5) nighttime O3 abundances in the secondary maximum were reduced by 10 %–30 %. The O3 profiles retrieved from the nominal mode (NOM) and the middle-atmosphere modes are fully consistent in their common altitude range (20–70 km). Only at 60–70 km does daytime O3 of NOM seem to be larger than that of MA/UA by 2 %–10 %. Compared to other satellite instruments, MIPAS seems to have a positive bias of 5 %–8 % below 70 km. Noticeably, the new version of MIPAS data agrees much better than before with all instruments in the upper mesosphere–lower thermosphere, reducing the differences from ∼± 20 % to ∼± 10 %. Further, the diurnal variation in O3 in the upper mesosphere (near 80 km) has been significantly improved.

Version 8 IMK–IAA MIPAS temperatures from 12–15 µm spectra: Middle and Upper Atmosphere modes

Abstract. Motivated by an improved European Space Agency (ESA) version of calibrated Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) spectra (version 8.03), we have released version 8 of MIPAS temperatures and pointing information retrieved from 2005–2012 MIPAS measurements at 12–15 µm in the Middle Atmosphere (MA), Upper Atmosphere (UA) and Noctilucent Cloud (NLC) measurement modes. The Institute of Meteorology and Climate Research–Instituto de Astrofisica de Andalucia (IMK–IAA) retrieval processor in use considers non-local thermodynamic equilibrium (non-LTE) emission explicitly for each limb scan. This non-LTE treatment is essential to obtain accurate temperatures above the mid-mesosphere because at the altitudes covered, up to 115 km, the simplified climatology-based non-LTE treatment employed for the Nominal (NOM) measurements is insufficient. Other updates in MA/UA/NLC version 8 non-LTE temperature retrievals from previous data releases include more realistic atomic oxygen and carbon dioxide abundances, an updated set of spectroscopic data, an improved spectral shift retrieval, a continuum retrieval extended to altitudes up to 58 km, consideration of an altitude-dependent radiance offset retrieval, the use of wider microwindows above 85 km to capture the offset, an improved accuracy in forward model calculations, new a priori temperature information, improved temperature horizontal gradient retrievals and the use of MIPAS version 5 interfering species where available. The resulting MIPAS MA/UA/NLC IMK–IAA temperature dataset is reliable for scientific analysis in the full measurement vertical range for the MA (18–102 km) and the NLC (39–102 km) observations and from 42 to 115 km for the UA observations. The random temperature errors, dominated by the instrumental noise, are typically less than 1 K below 60 km, 1–3 K at 60–70 km, 3–5 K at 70–90 km, 6–8 K at 90–100 km, 8–12 K at 100–105 km and 12–20 K at 105–115 km. Random pointing correction errors, also mainly arising from instrumental noise, are on average 50 m for tangent altitudes up to 60 km and decrease linearly to values smaller than 20 m for altitudes above 95 km. The vertical resolution is 3 km at altitudes below 50 km, 3–5 km at 50–70 km, 4–6 km at 70–90 km, 6–10 km at 90–100 km and 8–11 km at 100–115 km. The systematic errors in retrieved temperatures below 75 km are driven by uncertainties in the CO2 spectroscopic data and, above 80 km, by uncertainties in the non-LTE model parameters (including collisional rates and atomic oxygen abundance) and the CO2 abundance. These lead to systematic temperature errors of less than 0.7 K below 55 km, 1 K at 60–80 km, 1–2 K at 80–90 km, 3 K at 95 km, 6–8 K at 100 km, 10–20 K at 105 km and 20–30 K at 115 km. Systematic errors in the tangent altitude correction, mainly arising from CO2 spectroscopic uncertainties, are 250 m at 20 km, 200 m at 40–60 km, 100 m at 80 km and smaller than 50 m above 90 km. The consistency between the MA/UA/NLC and the NOM IMK–IAA datasets is excellent below 70 km (typical 0.5–1 K differences). The comparison of this temperature dataset with co-located Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) temperature measurements shows excellent agreement, with differences typically within 1.5 K below 90 km, 1–3 K at 90–95 km, 1–5 K at 95–100 km, 1–8 K at 100–105 km and 1–10 K above. The agreement with SABER improves with respect to previous MIPAS IMK–IAA data versions.

Impact of chlorine ion chemistry on ozone loss in the middle atmosphere during very large solar proton events

Abstract. Solar coronal mass ejections can accelerate charged particles, mostly protons, to high energies, causing solar proton events (SPEs). Such energetic particles can precipitate upon the Earth's atmosphere, mostly in polar regions because of geomagnetic shielding. Here, SPE-induced chlorine activation due to ion chemistry can occur, and the activated chlorine depletes ozone in the polar middle atmosphere. We use the state-of-the-art 1D stacked-box Exoplanetary Terrestrial Ion Chemistry (ExoTIC) model of atmospheric ion and neutral composition to investigate such events in the Northern Hemisphere (NH). The Halloween SPE that occurred in late October 2003 is used as a test field for our study. This event has been extensively studied before using different 3D models and satellite observations. Our main purpose is to use such a large event that has been recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the Environmental Satellite (ENVISAT) to evaluate the performance of the ion chemistry model. Sensitivity tests were carried out for different model settings with a focus on the chlorine species of HOCl and ClONO2 as well as O3 and reactive nitrogen, NOy. The model simulations were performed in the Northern Hemisphere at a high latitude of 67.5∘ N, inside the polar cap. Comparison of the simulated effects against MIPAS observations for the Halloween SPE revealed rather good temporal agreement, also in terms of altitude range for HOCl, O3 and NOy. For ClONO2, good agreement was found in terms of altitude range. The model showed ClONO2 enhancements after the peak of the event. The best model setting was the one with full ion chemistry where O(1D) was set to photo-chemical equilibrium. HOCl and ozone changes are very well reproduced by the model, especially for nighttime. HOCl was found to be the main active chlorine species under nighttime conditions, resulting in an increase of more than 0.2 ppbv. Further, ClONO2 enhancements of 0.2–0.3 ppbv have been observed during both daytime and nighttime. Model settings that compared best with MIPAS observations were applied to an extreme solar event that occurred in AD 775, presumably once in a 1000-year event. With the model applied to this scenario, an assessment can be made about what is to be expected at worst for the effects of a SPE on the middle atmosphere, concentrating on the effects of ion chemistry compared to crude parameterizations. Here, a systematic analysis comparing the impact of the Halloween SPE and the extreme event on the Earth's middle atmosphere is presented. As seen from the model simulations, both events were able to perturb the polar stratosphere and mesosphere with a high production of NOy and HOx. Longer-lasting and stronger stratospheric ozone loss was seen for the extreme event. A qualitative difference between the two events and a long-lasting impact on HOCl and HCl for the extreme event were found. Chlorine ion chemistry contributed to stratospheric ozone losses of 2.4 % for daytime and 10 % for nighttime during the Halloween SPE, as seen with time-dependent ionization rates applied to the model. Furthermore, while comparing the Halloween SPE and the extreme scenario, with ionization rate profiles applied just for the event day, the inclusion of chlorine ion chemistry added ozone losses of 10 % and 20 % respectively.

Validation of Version 1.3 Ozone Measured by the SOFIE Instrument

AbstractThe Solar Occultation for Ice Experiment (SOFIE) has operated aboard the Aeronomy of Ice in the Mesosphere (AIM) satellite since 2007. SOFIE uses solar occultation to retrieve ozone (O3) profiles from ∼20 to 100 km altitude, typically at polar latitudes. This study validates SOFIE O3 profiles, including error analysis and comparisons with independent observations. Comparisons are made to the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE‐FTS) and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) satellite instruments. SOFIE shows qualitative and quantitative agreement with both data sets between 30 and 70 km and better overall agreement in the northern hemisphere. SOFIE and ACE mean differences are typically within 20% in the 30–70 km altitude range. SOFIE and MIPAS exhibit mean difference values within 30% in the winter and 20% for all other seasons averaged, between ∼30 and 60 km. Seasonal comparisons indicate similar variations in both hemispheres and through all seasons. The comparisons indicate that SOFIE is biased 5%–10% low at 30–70 km altitudes, with greater differences at higher and lower altitudes. The comparisons are challenging due to the low O3 concentrations at high altitudes, the limited number of coincidences, and the large diurnal variation in mesospheric O3 during twilight hours.

Inferring the photolysis rate of NO2 in the stratosphere based on satellite observations

Abstract. NO and NO2 (NOx) play major roles in both tropospheric and stratospheric chemistry. This paper provides a novel method to obtain a global and accurate photolysis rate for NO2 based on satellite data. The photolysis rate J(NO2) dominates the daytime diurnal variation of NOx photochemistry. Here the spatial variation of J(NO2) at 50–90∘ S in December from 20–40 km is obtained using data from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) experiment. Because NO and NO2 rapidly exchange with one another in the daytime, J(NO2) can be attained assuming steady state, and the results are shown to be consistent with model results. The J(NO2) value decreases as the solar zenith angle increases and has a weak altitude dependence. A key finding is that satellite-derived J(NO2) increases in the polar regions, in good agreement with model predictions, due to the effects of ice and snow on surface albedo. Thus, the method presented here provides an observation-based check on the role of albedo in driving polar photochemistry.

Michelson Interferometer for Passive Atmospheric Sounding Institute of Meteorology and Climate Research/Instituto de Astrofísica de Andalucía version 8 retrieval of nitric oxide and lower-thermospheric temperature

Abstract. New global nitric oxide (NO) volume mixing ratio and lower-thermospheric temperature data products, retrieved from Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) spectra with the Institute of Meteorology and Climate Research and Instituto de Astrofísica de Andalucía (IMK-IAA) MIPAS data processor, have been released. The dataset covers the entire Envisat mission lifetime and includes retrieval results from all MIPAS observation modes. The data are based on European Space Agency (ESA) version 8 calibration and were processed using an improved retrieval approach compared to previous versions, specifically regarding the choice and construction of the a priori and atmospheric parameter profiles, the treatment of horizontal inhomogeneities, the treatment of the radiance offset correction, and the selection of optimized numerical settings. NO retrieval errors in individual observations are dominated by measurement noise and range from 5 % to 50 % in the stratosphere and thermosphere and reach 40 % to 90 % in the mesosphere. Systematic errors are typically within 10 %–30 %. Lower-thermospheric temperature errors are 5 to 50 K with a systematic component of around 20 K, the latter being dominated by non-thermodynamic equilibrium (non-LTE)-related uncertainties. NO data from different observation modes are consistent within 5 %–10 %. MIPAS version 8 temperatures have a better representation of the diurnal tide in the lower thermosphere compared to previous data versions. The new MIPAS temperatures are systematically warmer than results from the empirical US Naval Research Laboratory Mass Spectrometer Incoherent Scatter Radar (NRLMSIS) version 2.0 model by 30 to 80 K in the 100–120 km region and are colder above.

Updated merged SAGE-CCI-OMPS+ dataset for the evaluation of ozone trends in the stratosphere

Abstract. 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).

Version 8 IMK–IAA MIPAS ozone profiles: nominal observation mode

Abstract. A new global O3 data product retrieved from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) spectra with the IMK–IAA MIPAS data processor has been released. These data are based on ESA version 8 recalibrated radiance spectra with improved temporal stability. Changes in the level-2 processing with respect to previous data versions include the following: (1) the retrievals use improved temperature data and thus suffer less from the propagation of related errors. (2) The background continuum is now considered up to 58 km. (3) A priori information is now used to constrain the retrieval of the radiance offset. (4) Water vapour is fitted jointly with ozone to minimize the impact of interfering water lines. (5) A more adequate regularization has been chosen. (6) Ozone absorption lines in the MIPAS A band (685–980 cm−1) are used almost exclusively because of inconsistencies in spectroscopic data in the MIPAS AB band (1010–1180 cm−1). Only at altitudes above 50 km, where A-band ozone lines do not provide sufficient information, are ozone lines in the MIPAS AB band used. (7) Temperature-adjusted climatologies of vibrational temperatures of O3 and CO2 are considered to account for non-local thermodynamic equilibrium radiation. Ozone errors are estimated to be less than 10 % in the altitude range 20–50 km. The error budget is dominated by the spectroscopic errors, followed by the uncertainty of the instrumental line shape function, the gain calibration error, and the spectral noise. The error contribution of interfering gases is almost negligible. The vertical resolution depends on altitude and atmospheric conditions. In 2002–2004 it varies between 2.5 km at the lowest altitudes and 6 km at 70 km, while in 2005–2012 it covers 2 to 5.5 km in the same altitude range. The horizontal smearing in terms of the full width at half maximum of the horizontal component of the two-dimensional averaging kernel matrix is smaller than, or approximately equal to, the distance between two subsequent limb scans at all altitudes. This implies that the horizontal resolution is sampling-limited or optimal, respectively. An additional data version is made available that is free of the formal a priori information and thus more user-friendly for certain applications. Version 8 ozone results show a better consistency between the two MIPAS measurement periods. They seem to be more realistic than preceding data versions in terms of long-term stability, as at least a part of the drift is corrected. Further, the representation of elevated stratopause situations is improved.

Retrieval of atmospheric trace gases from satellite infrared limb sounding data

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument which operated in the near-to-mid infrared on the Envisat satellite from 2002–2012 is a Fourier-transform spectrometer for the measurement of high-resolution atmospheric emission spectra at the Earth’s limb. The initial operational products are profiles of temperature, H2O, O3, CH4, N2O, HNO3, and NO2, and this list is extended to include the important GHG (greenhouse gases) and ODS (ozone depleting substances) species using MORSE (orbital retrieval processor). This paper discusses retrievals of minor trace species of HCFC-22, HOCl, OCS, C2H6, COF2, HCN, CF4, SF6, and CCl4. Preliminary zonal mean results of these retrievals are satisfactory except for HCN and CF4 species. We then use MIPAS to estimate the total F and Cl budget in the atmosphere. Comparisons with SLIMCAT are also discussed, with the results consistent. Finally, we focus on improving the retrieval method for minor trace species, COF2, by adjusting correlation length and a priori constraint, as well as the chi-square method introduced to analyze noise. Tests have shown that our improvement could get more information from the measurements.

TUNER-compliant error estimation for MIPAS: methodology

Abstract. This paper describes the error estimation for temperature and trace gas mixing ratios retrieved from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) limb emission spectra. The following error sources are taken into account: measurement noise, propagated temperature and pointing noise, uncertainties in the abundances of spectrally interfering species, instrument line shape errors, and spectroscopic data uncertainties in terms of line intensities and broadening coefficients. Furthermore, both the direct impact of volatile and persistent gain calibration uncertainties, offset calibration, and spectral calibration uncertainties, as well as their impact through propagated calibration-related temperature and pointing uncertainties, are considered. An error source specific to the MIPAS upper atmospheric observation mode is the propagation of the smoothing error crosstalk of the combined NO and temperature retrieval. Whenever non-local thermodynamic equilibrium modelling is used in the retrieval, related kinetic constants and mixing ratios of species involved in the modelling of populations of excitational states also contribute to the error budget. Both generalized Gaussian error propagation and perturbation studies are used to estimate the error components. Error correlations are taken into account. Estimated uncertainties are provided for a multitude of atmospheric conditions. Some error sources were found to contribute both to the random and the systematic component of the total estimated error. The sequential nature of the MIPAS retrievals gives rise to entangled errors. These are caused by error sources that affect the uncertainty in the final data product via multiple pathways, i.e., on the one hand, directly, and, on the other hand, via errors caused in a preceding retrieval step. These errors tend to partly compensate for each other. The hard-to-quantify effect of the horizontally non-homogeneous atmosphere and unknown error correlations of spectroscopic data are considered to be the major limitations of the MIPAS error estimation.

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

Abstract. 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.

An optimal estimation-based retrieval of upper atmospheric oxygen airglow and temperature from SCIAMACHY limb observations

Abstract. An optimal estimation-based algorithm is developed to retrieve the number density of excited oxygen (O2) molecules that generate airglow emissions near 0.76 µm (b1Σg+ or A band) and 1.27 µm (a1Δg or 1Δ band) in the upper atmosphere. Both oxygen bands are important for the remote sensing of greenhouse gases. The algorithm is applied to the limb spectra observed by the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) instrument in both the nominal (tangent heights below ∼ 90 km) and mesosphere–lower thermosphere (MLT) modes (tangent heights spanning 50–150 km). The number densities of emitting O2 in the a1Δg band are retrieved in an altitude range of 25–100 km near-daily in 2010, providing a climatology of O2 a1Δg-band airglow emission. This climatology will help disentangle the airglow from backscattered light in nadir remote sensing of the a1Δg band. The global monthly distributions of the vertical column density of emitting O2 in a1Δg state show mainly latitudinal dependence without other discernible geographical patterns. Temperature profiles are retrieved simultaneously from the spectral shapes of the a1Δg-band airglow emission in the nominal limb mode (valid altitude range of 40–100 km) and from both a1Δg- and b1Σg+-band airglow emissions in the MLT mode (valid range of 60–105 km). The temperature retrievals from both airglow bands are consistent internally and in agreement with independent observations from the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), with the absolute mean bias near or below 5 K and root mean squared error (RMSE) near or below 10 K. The retrieved emitting O2 number density and temperature provide a unique dataset for the remote sensing of greenhouse gases and constraining the chemical and physical processes in the upper atmosphere.

Synergy of Using Nadir and Limb Instruments for Tropospheric Ozone Monitoring (SUNLIT)

Abstract. Satellite measurements in nadir and limb viewing geometry provide a complementary view of the atmosphere. An effective combination of the limb and nadir measurements can give new information about atmospheric composition. In this work, we present tropospheric ozone column datasets that have been created using a combination of total ozone columns from OMI (Ozone Monitoring Instrument) and TROPOMI (TROPOspheric Monitoring Instrument) with stratospheric ozone column datasets from several available limb-viewing instruments: MLS (Microwave Limb Sounder), OSIRIS (Optical Spectrograph and InfraRed Imaging System), MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), SCIAMACHY (SCanning Imaging Spectrometer for Atmospheric CHartographY), OMPS-LP (Ozone Mapping and Profiles Suite – Limb Profiler), and GOMOS (Global Ozone Monitoring by Occultation of Stars). We have developed further the methodological aspects of the assessment of tropospheric ozone using the residual method supported by simulations with the chemistry transport model SILAM (System for Integrated modeLling of Atmospheric coMposition). It has been shown that the accurate assessment of ozone in the upper troposphere and the lower stratosphere (UTLS) is of high importance for detecting the ground-level ozone patterns. The stratospheric ozone column is derived from a combination of ozone profiles from several satellite instruments in limb-viewing geometry. We developed a method for the data homogenization, which includes the removal of biases and a posteriori estimation of random uncertainties, thus making the data from different instruments compatible with each other. The high-horizontal- and vertical-resolution dataset of ozone profiles is created via interpolation of the limb profiles from each day to a 1∘×1∘ horizonal grid. A new kriging-type interpolation method, which takes into account data uncertainties and the information about natural ozone variations from the SILAM-adjusted ozone field, has been developed. To mitigate the limited accuracy and coverage of the limb profile data in the UTLS, a smooth transition to the model data is applied below the tropopause. This allows for the estimation of the stratospheric ozone column with full coverage of the UTLS. The derived ozone profiles are in very good agreement with collocated ozonesonde measurements. The residual method was successfully applied to OMI and TROPOMI clear-sky total ozone data in combination with the stratospheric ozone column from the developed high-resolution limb profile dataset. The resulting tropospheric ozone column is in very good agreement with other satellite data. The global distributions of tropospheric ozone exhibit enhancements associated with the regions of high tropospheric ozone production. The main datasets created are (i) a monthly 1∘×1∘ global tropospheric ozone column dataset (from ground to 3 km below the tropopause) using OMI and limb instruments, (ii) a monthly 1∘×1∘ global tropospheric ozone column dataset using TROPOMI and limb instruments, and (iii) a daily 1∘×1∘ interpolated stratospheric ozone column from limb instruments. Other datasets, which are created as an intermediate step of creating the tropospheric ozone column data, are (i) a daily 1∘×1∘ clear-sky and total ozone column from OMI and TROPOMI, (ii) a daily 1∘×1∘ homogenized and interpolated dataset of ozone profiles from limb instruments, and (iii) a daily 1∘×1∘ dataset of ozone profiles from SILAM simulations with adjustment to satellite data. These datasets can be used in various studies related to variability and trends in ozone distributions in both the troposphere and the stratosphere. The datasets are processed from the beginning of OMI and TROPOMI measurements until December 2020 and are planned to be regularly extended in the future.

Level 2 processor and auxiliary data for ESA Version 8 final full mission analysis of MIPAS measurements on ENVISAT

Abstract. High quality long-term data sets of altitude-resolved measurements of the atmospheric composition are important because they can be used both to study the evolution of the atmosphere and as a benchmark for future missions. For the final ESA reprocessing of MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) on ENVISAT (ENViromental SATellite) data, numerous improvements were implemented in the Level 2 (L2) processor Optimised Retrieval Model (ORM) version 8.22 (V8) and its auxiliary data. The implemented changes involve all aspects of the processing chain, from the modelling of the measurements with the handling of the horizontal inhomogeneities along the line of sight to the use of the optimal estimation technique to retrieve the minor species, from a more sensitive approach to detecting the spectra affected by clouds to a refined method for identifying low quality products. Improvements in the modelling of the measurements were also obtained with an update of the used spectroscopic data and of the databases providing the a priori knowledge of the atmosphere. The HITRAN_mipas_pf4.45 spectroscopic database was finalised with new spectroscopic data verified with MIPAS measurements themselves, while recently measured cross-sections were used for the heavy molecules. The Level 2 Initial Guess (IG2) data set, containing the climatology used by the MIPAS L2 processor to generate the initial guess and interfering species profiles when the retrieved profiles from previous scans are not available, was improved taking into account the diurnal variation of the profiles defined using climatologies from both measurements and models. Horizontal gradients were generated using the ECMWF ERA-Interim data closest in time and space to the MIPAS data. Further improvements in the L2 V8 products derived from the use of the L1b V8 products, which were upgraded to reduce the instrumental temporal drift and to handle the abrupt changes in the calibration gain. The improvements introduced into the ORM V8 L2 processor and its upgraded auxiliary data, together with the use of the L1b V8 products, lead to the generation of the MIPAS L2 V8 products, which are characterised by an increased accuracy, better temporal stability and a greater number of retrieved species.

The impact of sulfur hexafluoride (SF<sub>6</sub>) sinks on age of air climatologies and trends

Abstract. Mean age of air (AoA) is a common diagnostic for the strength of the stratospheric overturning circulation in both climate models and observations. AoA climatologies and AoA trends over the recent decades of model simulations and proxies derived from observations of long-lived tracers do not agree. Satellite observations show much older air than climate models, and while most models compute a clear decrease in AoA over the last decades, a 30-year time series from measurements shows a statistically nonsignificant positive trend in the Northern Hemisphere extratropical middle stratosphere. Measurement-based AoA derivations are often founded on observations of the trace gas sulfur hexafluoride (SF6), a fairly long-lived gas with a near-linear increase in emissions during recent decades. However, SF6 has chemical sinks in the mesosphere that are not considered in most model studies. In this study, we explicitly compute the chemical SF6 sinks based on chemical processes in the global chemistry climate model EMAC (ECHAM/MESSy Atmospheric Chemistry). We show that good agreement between stratospheric AoA in EMAC and MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) is reached through the inclusion of chemical SF6 sinks, as these sinks lead to a strong increase in the stratospheric AoA and, therefore, to a better agreement with MIPAS satellite observations. Remaining larger differences at high latitudes are addressed, and possible reasons for these differences are discussed. Subsequently, we demonstrate that the AoA trends are also strongly influenced by the chemical SF6 sinks. Under consideration of the SF6 sinks, the AoA trends over the recent decades reverse sign from negative to positive. We conduct sensitivity simulations which reveal that this sign reversal does not result from trends in the stratospheric circulation strength nor from changes in the strength of the SF6 sinks. We illustrate that even a constant SF6 destruction rate causes a positive trend in the derived AoA, as the amount of depleted SF6 scales with increasing SF6 abundance itself. In our simulations, this effect overcompensates for the impact of the accelerating stratospheric circulation which naturally decreases AoA. Although various sources of uncertainties cannot be quantified in detail in this study, our results suggest that the inclusion of SF6 depletion in models has the potential to reconcile the AoA trends of models and observations. We conclude the study with a first approach towards a correction to account for SF6 loss and deduce that a linear correction might be applicable to values of AoA of up to 4 years.

The ESA MIPAS/Envisat level2-v8 dataset: 10 years of measurements retrieved with ORM v8.22

Abstract. The observations acquired during the full mission of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, aboard the European Space Agency Environmental Satellite (Envisat), have been analysed with version 8.22 of the Optimised Retrieval Model (ORM), originally developed as the scientific prototype of the ESA level-2 processor for MIPAS observations. The results of the analyses have been included into the MIPAS level-2 version 8 (level2-v8) database containing atmospheric fields of pressure, temperature, and volume mixing ratio (VMR) of MIPAS main targets H2O, O3, HNO3, CH4, N2O, and NO2, along with the minor gases CFC-11, ClONO2, N2O5, CFC-12, COF2, CCl4, CF4, HCFC-22, C2H2, CH3Cl, COCl2, C2H6, OCS, and HDO. The database covers all the measurements acquired by MIPAS in the nominal measurement mode of the full resolution (FR) part of the mission (from July 2002 to March 2004) and all the observation modes of the optimised resolution (OR) part (from January 2005 to April 2012). The number of species included in the MIPAS level2-v8 dataset makes it of particular importance for the studies of stratospheric chemistry. The database is considered by ESA the final release of the MIPAS level-2 products. The ORM algorithm is operated at the vertical grid coincident to the tangent altitudes of the observations or to a subset of them, spanning (in the nominal mode) the altitude range from 6 to 68 km in the FR phase and from 6 to 70 km in the OR period. In the latitude domain, FR profiles are spaced by about 4.7∘, while the OR profiles are spaced by about 3.7∘. For each retrieved species, the auxiliary data and the retrieval choices are described. Each product is characterised in terms of the retrieval error, spatial resolution, and “useful” vertical range in both phases of the MIPAS mission. These depend on the characteristics of the measurements (spectral and vertical resolution of the measurements), the retrieval choices (number of spectral points included in the analyses, number of altitudes included in the vertical retrieval grid), and the information content of the measurements for each trace species. For temperature, water vapour, ozone, and nitric acid, the number of degrees of freedom is significantly larger in the OR phase than in the FR one, mainly due to the finer vertical measurement grid. In the FR phase, some trace species are characterised by a smaller retrieval error with respect to the OR phase, mainly due to the larger number of spectral points used in the analyses, along with the reduced vertical resolution. The way of handling possible caveats (negative VMR, vertical grid representation) is discussed. The quality of the retrieved profiles is assessed through four criteria, two providing information on the successful convergence of the retrieval iterations, one on the capability of the retrieval to reproduce the measurements, and one on the presence of outliers. An easy way to identify and filter the problematic profiles with the information contained in the output files is provided. MIPAS level2-v8 data are available to the scientific community through the ESA portal (https://doi.org/10.5270/EN1-c8hgqx4).

Phosgene distribution derived from MIPAS ESA v8 data: intercomparisons and trends

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) measured the middle-infrared limb emission spectrum of the atmosphere from 2002 to 2012 on board ENVISAT, a polar-orbiting satellite. Recently, the European Space Agency (ESA) completed the final reprocessing of MIPAS measurements, using version 8 of the level 1 and level 2 processors, which include more accurate models, processing strategies, and auxiliary data. The list of retrieved gases has been extended, and it now includes a number of new species with weak emission features in the MIPAS spectral range. The new retrieved trace species include carbonyl chloride (COCl2), also called phosgene. Due to its toxicity, its use has been reduced over the years; however, it is still used by chemical industries for several applications. Besides its direct injection in the troposphere, stratospheric phosgene is mainly produced from the photolysis of CCl4, a molecule present in the atmosphere because of human activity. Since phosgene has a long stratospheric lifetime, it must be carefully monitored as it is involved in the ozone destruction cycles, especially over the winter polar regions. In this paper we exploit the ESA MIPAS version 8 data in order to discuss the phosgene distribution, variability, and trends in the middle and lower stratosphere and in the upper troposphere. The zonal averages show that phosgene volume mixing ratio is larger in the stratosphere, with a peak of 40 pptv (parts per trillion by volume) between 50 and 30 hPa at equatorial latitudes, while at middle and polar latitudes it varies from 10 to 25 pptv. A moderate seasonal variability is observed in polar regions, mostly between 80 and 50 hPa. The comparison of MIPAS–ENVISAT COCl2 v8 profiles with the ones retrieved from MIPAS balloon and ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) measurements highlights a negative bias of about 2 pptv, mainly in polar and mid-latitude regions. Part of this bias is attributed to the fact that the ESA level 2 v8 processor uses an updated spectroscopic database. For the trend computation, a fixed pressure grid is used to interpolate the phosgene profiles, and, for each pressure level, VMR (volume mixing ratio) monthly averages are computed in pre-defined 10∘ wide latitude bins. Then, for each latitudinal bin and pressure level, a regression model has been fitted to the resulting time series in order to derive the atmospheric trends. We find that the phosgene trends are different in the two hemispheres. The analysis shows that the stratosphere of the Northern Hemisphere is characterized by a negative trend of about −7 pptv per decade, while in the Southern Hemisphere phosgene mixing ratios increase with a rate of the order of +4 pptv per decade. This behavior resembles the stratospheric trend of CCl4, which is the main stratospheric source of COCl2. In the upper troposphere a positive trend is found in both hemispheres.

The Michelson Interferometer for Passive Atmospheric Sounding global climatology of BrONO<sub>2</sub> 2002–2012: a test for stratospheric bromine chemistry

Abstract. We present the first observational dataset of vertically resolved global stratospheric BrONO2 distributions from July 2002 until April 2012 and compare them to results of the atmospheric chemical climate model ECHAM/MESSy Atmospheric Chemistry (EMAC). The retrieved distributions are based on space-borne measurements of infrared limb-emission spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat. The derived vertical profiles of BrONO2 volume mixing ratios represent 10∘ latitude bins and 3 d means, separated into sunlit observations and observations in the dark. The estimated uncertainties are around 1–4 pptv, caused by spectral noise for single profiles as well as for further parameter and systematic errors which may not improve by averaging. Vertical resolutions range from 3 to 8 km between 15 and 35 km altitude. All leading modes of spatial and temporal variability of stratospheric BrONO2 in the observations are well replicated by the model simulations: the large diurnal variability, the low values during polar winter as well as the maximum values at mid and high latitudes during summer. Three major differences between observations and model results are observed: (1) a model underestimation of enhanced BrONO2 in the polar winter stratosphere above about 30 km of up to 15 pptv, (2) up to 8 pptv higher modelled values than observed globally in the lower stratosphere up to 25 km, most obvious during night, and (3) up to 5 pptv lower modelled concentrations at tropical latitudes between 27 and 32 km during sunlit conditions. (1) is explained by the model missing enhanced NOx produced in the mesosphere and lower thermosphere subsiding at high latitudes in winter. This is the first time that observational evidence for enhancement of BrONO2 caused by mesospheric NOx production is reported. The other major inconsistencies (2, 3) between EMAC model results and observations are studied by sensitivity runs with a 1D model. These tentatively hint at a model underestimation of heterogeneous loss of BrONO2 in the lower stratosphere, a simulated production of BrONO2 that is too low during the day as well as strongly underestimated BrONO2 volume mixing ratios when loss via reaction with O(3P) is considered in addition to photolysis. However, considering the uncertainty ranges of model parameters and of measurements, an unambiguous identification of the causes of the differences remains difficult. The observations have also been used to derive the total stratospheric bromine content relative to years of stratospheric entry between 1997 and 2007. With an average value of 21.2±1.4 pptv of Bry at mid latitudes where the modelled adjustment from BrONO2 to Bry is smallest, the MIPAS data agree with estimates of Bry derived from observations of BrO as well as from MIPAS-Balloon measurements of BrONO2.