Michelson Interferometer For Passive Atmospheric Sounding Research Articles

Comparison of the GOSAT TANSO-FTS TIR CH<sub>4</sub> volume mixing ratio vertical profiles with those measured by ACE-FTS, ESA MIPAS, IMK-IAA MIPAS, and 16 NDACC stations

Abstract. The primary instrument on the Greenhouse gases Observing SATellite (GOSAT) is the Thermal And Near infrared Sensor for carbon Observations (TANSO) Fourier transform spectrometer (FTS). TANSO-FTS uses three short-wave infrared (SWIR) bands to retrieve total columns of CO2 and CH4 along its optical line of sight and one thermal infrared (TIR) channel to retrieve vertical profiles of CO2 and CH4 volume mixing ratios (VMRs) in the troposphere. We examine version 1 of the TANSO-FTS TIR CH4 product by comparing co-located CH4 VMR vertical profiles from two other remote-sensing FTS systems: the Canadian Space Agency's Atmospheric Chemistry Experiment FTS (ACE-FTS) on SCISAT (version 3.5) and the European Space Agency's Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat (ESA ML2PP version 6 and IMK-IAA reduced-resolution version V5R_CH4_224/225), as well as 16 ground stations with the Network for the Detection of Atmospheric Composition Change (NDACC). This work follows an initial inter-comparison study over the Arctic, which incorporated a ground-based FTS at the Polar Environment Atmospheric Research Laboratory (PEARL) at Eureka, Canada, and focuses on tropospheric and lower-stratospheric measurements made at middle and tropical latitudes between 2009 and 2013 (mid-2012 for MIPAS). For comparison, vertical profiles from all instruments are interpolated onto a common pressure grid, and smoothing is applied to ACE-FTS, MIPAS, and NDACC vertical profiles. Smoothing is needed to account for differences between the vertical resolution of each instrument and differences in the dependence on a priori profiles. The smoothing operators use the TANSO-FTS a priori and averaging kernels in all cases. We present zonally averaged mean CH4 differences between each instrument and TANSO-FTS with and without smoothing, and we examine their information content, their sensitive altitude range, their correlation, their a priori dependence, and the variability within each data set. Partial columns are calculated from the VMR vertical profiles, and their correlations are examined. We find that the TANSO-FTS vertical profiles agree with the ACE-FTS and both MIPAS retrievals' vertical profiles within 4 % (± ∼ 40 ppbv) below 15 km when smoothing is applied to the profiles from instruments with finer vertical resolution but that the relative differences can increase to on the order of 25 % when no smoothing is applied. Computed partial columns are tightly correlated for each pair of data sets. We investigate whether the difference between TANSO-FTS and other CH4 VMR data products varies with latitude. Our study reveals a small dependence of around 0.1 % per 10 degrees latitude, with smaller differences over the tropics and greater differences towards the poles.

CCl<sub>4</sub> distribution derived from MIPAS ESA v7 data: intercomparisons, trend, and lifetime estimation

Abstract. Atmospheric emissions of carbon tetrachloride (CCl4) are regulated by the Montreal Protocol due to its role as a strong ozone-depleting substance. The molecule has been the subject of recent increased interest as a consequence of the so-called mystery of CCl4, the discrepancy between atmospheric observations and reported production and consumption. Surface measurements of CCl4 atmospheric concentrations have declined at a rate almost 3 times lower than its lifetime-limited rate, suggesting persistent atmospheric emissions despite the ban. In this paper, we study CCl4 vertical and zonal distributions in the upper troposphere and lower stratosphere (including the photolytic loss region, 70–20 hPa), its trend, and its stratospheric lifetime using measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), which operated onboard the ENVISAT satellite from 2002 to 2012. Specifically, we use the MIPAS data product generated with Version 7 of the Level 2 algorithm operated by the European Space Agency.The CCl4 zonal means show features typical of long-lived species of anthropogenic origin that are destroyed primarily in the stratosphere, with larger quantities in the troposphere and a monotonic decrease with increasing altitude in the stratosphere. MIPAS CCl4 measurements have been compared with independent measurements from other satellite and balloon-borne remote sounders, showing a good agreement between the different datasets.CCl4 trends are calculated as a function of both latitude and altitude. Negative trends of about −10 to −15 pptv decade−1 (−10 to −30 % decade−1) are found at all latitudes in the upper troposphere–lower stratosphere region, apart from a region in the southern midlatitudes between 50 and 10 hPa where the trend is positive with values around 5–10 pptv decade−1 (15–20 % decade−1). At the lowest altitudes sounded by MIPAS, we find trends consistent with those determined on the basis of long-term ground-based measurements (−10 to −13 pptv decade−1). For higher altitudes, the trend shows a pronounced asymmetry between the Northern and Southern hemispheres, and the magnitude of the decline rate increases with altitude. We use a simplified model assuming tracer–tracer linear correlations to determine CCl4 lifetime in the lower stratosphere. The calculation provides a global average lifetime of 47 (39–61) years, considering CFC-11 as the reference tracer. This value is consistent with the most recent literature result of 44 (36–58) years.

Validation of the MIPAS CO2 volume mixing ratio in the mesosphere and lower thermosphere and comparison with WACCM simulations

AbstractWe present the validation of Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) CO2 daytime concentration in the mesosphere and lower thermosphere by comparing with Atmospheric Chemistry Experiment (ACE) Fourier transform spectrometer and Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) data. MIPAS shows a very good agreement with ACE below 100 km with differences of ∼5%. Above 100 km, MIPAS CO2 is generally lower than ACE with differences growing from ∼5% at 100 km to 20–40% near 110–120 km. Part of this disagreement can be explained by the lack of a nonlocal thermodynamic equilibrium correction in ACE. MIPAS also agrees very well (∼5%) with SABER below 100 km. At 90–105 km, MIPAS is generally smaller than SABER by 10–30% in the polar summers. At 100–120 km, MIPAS and SABER CO2 agree within ∼10% during equinox but, for solstice, MIPAS is larger by 10–25%, except near the polar summer. Whole Atmosphere Community Climate Model (WACCM) CO2 shows the major MIPAS features. At 75–100 km, the agreement is very good (∼5%), with maximum differences of ∼10%. At 95–115 km MIPAS CO2 is larger than WACCM by 20–30% in the winter hemisphere but smaller (20–40%) in the summer. Above 95–100 km WACCM generally overestimates MIPAS CO2 by about 20–80% except in the polar summer where underestimates it by 20–40%. MIPAS CO2 favors a large eddy diffusion below 100 km and suggests that the meridional circulation of the lower thermosphere is stronger than in WACCM. The three instruments and WACCM show a clear increase of CO2 with time, more markedly at 90–100 km.

Effect of volcanic aerosol on stratospheric NO<sub>2</sub> and N<sub>2</sub>O<sub>5</sub> from 2002–2014 as measured by Odin-OSIRIS and Envisat-MIPAS

Abstract. Following the large volcanic eruptions of Pinatubo in 1991 and El Chichón in 1982, decreases in stratospheric NO2 associated with enhanced aerosol were observed. The Optical Spectrograph and Infrared Imaging Spectrometer (OSIRIS) measured the widespread enhancements of stratospheric aerosol following seven volcanic eruptions between 2002 and 2014, although the magnitudes of these eruptions were all much smaller than the Pinatubo and El Chichón eruptions. In order to isolate and quantify the relationship between volcanic aerosol and NO2, NO2 anomalies were calculated using measurements from OSIRIS and the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). In the tropics, variability due to the quasi-biennial oscillation was subtracted from the time series. OSIRIS profile measurements indicate that the strongest anticorrelations between NO2 and volcanic aerosol extinction were for the 5 km layer starting ∼ 3 km above the climatological mean tropopause at the given latitude. OSIRIS stratospheric NO2 partial columns in this layer were found to be smaller than background NO2 levels during these aerosol enhancements by up to ∼ 60 % with typical Pearson correlation coefficients of R ∼ −0. 7. MIPAS also observed decreases in NO2 partial columns during periods affected by volcanic aerosol, with percent differences of up to ∼ 25 % relative to background levels. An even stronger anticorrelation was observed between OSIRIS aerosol optical depth and MIPAS N2O5 partial columns, with R ∼ −0. 9, although no link with MIPAS HNO3 was observed. The variation in OSIRIS NO2 with increasing aerosol was found to be consistent with simulations from a photochemical box model within the estimated model uncertainty.

Merged ozone profiles from four MIPAS processors

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) was an infrared (IR) limb emission spectrometer on the Envisat platform. Currently, there are four MIPAS ozone data products, including the operational Level-2 ozone product processed at ESA, with the scientific prototype processor being operated at IFAC Florence, and three independent research products developed by the Istituto di Fisica Applicata Nello Carrara (ISAC-CNR)/University of Bologna, Oxford University, and the Karlsruhe Institute of Technology–Institute of Meteorology and Climate Research/Instituto de Astrofísica de Andalucía (KIT–IMK/IAA). Here we present a dataset of ozone vertical profiles obtained by merging ozone retrievals from four independent Level-2 MIPAS processors. We also discuss the advantages and the shortcomings of this merged product. As the four processors retrieve ozone in different parts of the spectra (microwindows), the source measurements can be considered as nearly independent with respect to measurement noise. Hence, the information content of the merged product is greater and the precision is better than those of any parent (source) dataset. The merging is performed on a profile per profile basis. Parent ozone profiles are weighted based on the corresponding error covariance matrices; the error correlations between different profile levels are taken into account. The intercorrelations between the processors' errors are evaluated statistically and are used in the merging. The height range of the merged product is 20–55 km, and error covariance matrices are provided as diagnostics. Validation of the merged dataset is performed by comparison with ozone profiles from ACE-FTS (Atmospheric Chemistry Experiment–Fourier Transform Spectrometer) and MLS (Microwave Limb Sounder). Even though the merging is not supposed to remove the biases of the parent datasets, around the ozone volume mixing ratio peak the merged product is found to have a smaller (up to 0.1 ppmv) bias with respect to ACE-FTS than any of the parent datasets. The bias with respect to MLS is of the order of 0.15 ppmv at 20–30 km height and up to 0.45 ppmv at larger altitudes. The agreement between the merged data MIPAS dataset with ACE-FTS is better than that with MLS. This is, however, the case for all parent processors as well.

A decadal satellite record of gravity wave activity in the lower stratosphere to study polar stratospheric cloud formation

Abstract. Atmospheric gravity waves yield substantial small-scale temperature fluctuations that can trigger the formation of polar stratospheric clouds (PSCs). This paper introduces a new satellite record of gravity wave activity in the polar lower stratosphere to investigate this process. The record is comprised of observations of the Atmospheric Infrared Sounder (AIRS) aboard NASA's Aqua satellite from January 2003 to December 2012. Gravity wave activity is measured in terms of detrended and noise-corrected 15 µm brightness temperature variances, which are calculated from AIRS channels that are the most sensitive to temperature fluctuations at about 17–32 km of altitude. The analysis of temporal patterns in the data set revealed a strong seasonal cycle in wave activity with wintertime maxima at mid- and high latitudes. The analysis of spatial patterns indicated that orography as well as jet and storm sources are the main causes of the observed waves. Wave activity is closely correlated with 30 hPa zonal winds, which is attributed to the AIRS observational filter. We used the new data set to evaluate explicitly resolved temperature fluctuations due to gravity waves in the European Centre for Medium-Range Weather Forecasts (ECMWF) operational analysis. It was found that the analysis reproduces orographic and non-orographic wave patterns in the right places, but that wave amplitudes are typically underestimated by a factor of 2–3. Furthermore, in a first survey of joint AIRS and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) satellite observations, nearly 50 gravity-wave-induced PSC formation events were identified. The survey shows that the new AIRS data set can help to better identify such events and more generally highlights the importance of the process for polar ozone chemistry.

Global carbonyl sulfide (OCS) measured by MIPAS/Envisat during 2002–2012

Abstract. We present a global carbonyl sulfide (OCS) data set covering the period June 2002 to April 2012, derived from FTIR (Fourier transform infrared) limb emission spectra measured with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on the ENVISAT satellite. The vertical resolution is 4–5 km in the height region 6–15 km and 15 at 40 km altitude. The total estimated error amounts to 40–50 pptv between 10 and 20 km and to 120 pptv at 40 km altitude. MIPAS OCS data show no systematic bias with respect to balloon observations, with deviations mostly below ±50 pptv. However, they are systematically higher than the OCS volume mixing ratios of the ACE-FTS instrument on SCISAT, with maximum deviations of up to 100 pptv in the altitude region 13–16 km. The data set of MIPAS OCS exhibits only moderate interannual variations and low interhemispheric differences. Average concentrations at 10 km altitude range from 480 pptv at high latitudes to 500–510 pptv in the tropics and at northern mid-latitudes. Seasonal variations at 10 km altitude amount to up to 35 pptv in the Northern and up to 15 pptv in the Southern Hemisphere. Northern hemispheric OCS abundances at 10 km altitude peak in June in the tropics and around October at high latitudes, while the respective southern hemispheric maxima were observed in July and in November. Global OCS distributions at 250 hPa (∼ 10–11 km) show enhanced values at low latitudes, peaking during boreal summer above the western Pacific and the Indian Ocean, which indicates oceanic release. Further, a region of depleted OCS amounts extending from Brazil to central and southern Africa was detected at this altitude, which is most pronounced in austral summer. This depletion is related to seasonally varying vegetative uptake by the tropical forests. Typical signatures of biomass burning like the southern hemispheric biomass burning plume are not visible in MIPAS data, indicating that this process is only a minor source of upper tropospheric OCS. At the 150 hPa level (∼ 13–14 km) enhanced amounts of OCS were also observed inside the Asian monsoon anticyclone, but this enhancement is not especially outstanding compared to other low latitude regions at the same altitude. At the 80 hPa level (∼ 17–18 km), equatorward transport of mid-latitude air masses containing lower OCS amounts around the summertime anticyclones was observed. A significant trend could not be detected in upper tropospheric MIPAS OCS amounts, which points to globally balanced sources and sinks. Simulations with the ECHAM-MESSy model reproduce the observed latitudinal cross sections fairly well.

Global distributions of CO<sub>2</sub> volume mixing ratio in the middle and upper atmosphere from daytime MIPAS high-resolution spectra

Abstract. Global distributions of the CO2 vmr (volume mixing ratio) in the mesosphere and lower thermosphere (from 70 up to ∼ 140 km) have been derived from high-resolution limb emission daytime MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) spectra in the 4.3 µm region. This is the first time that the CO2 vmr has been retrieved in the 120–140 km range. The data set spans from January 2005 to March 2012. The retrieval of CO2 has been performed jointly with the elevation pointing of the line of sight (LOS) by using a non-local thermodynamic equilibrium (non-LTE) retrieval scheme. The non-LTE model incorporates the new vibrational–vibrational and vibrational–translational collisional rates recently derived from the MIPAS spectra by [Jurado-Navarro et al.(2015)]. It also takes advantage of simultaneous MIPAS measurements of other atmospheric parameters (retrieved in previous steps), such as the kinetic temperature (derived up to ∼ 100 km from the CO2 15 µm region of MIPAS spectra and from 100 up to 170 km from the NO 5.3 µm emission of the same MIPAS spectra) and the O3 measurements (up to ∼ 100 km). The latter is very important for calculations of the non-LTE populations because it strongly constrains the O(3P) and O(1D) concentrations below ∼ 100 km. The estimated precision of the retrieved CO2 vmr profiles varies with altitude ranging from ∼ 1 % below 90 km to 5 % around 120 km and larger than 10 % above 130 km. There are some latitudinal and seasonal variations of the precision, which are mainly driven by the solar illumination conditions. The retrieved CO2 profiles have a vertical resolution of about 5–7 km below 120 km and between 10 and 20 km at 120–140 km. We have shown that the inclusion of the LOS as joint fit parameter improves the retrieval of CO2, allowing for a clear discrimination between the information on CO2 concentration and the LOS and also leading to significantly smaller systematic errors. The retrieved CO2 has an improved accuracy because of the new rate coefficients recently derived from MIPAS and the simultaneous MIPAS measurements of other key atmospheric parameters (retrieved in previous steps) needed for non-LTE modelling like kinetic temperature and O3 concentration. The major systematic error source is the uncertainty of the pressure/temperature profiles, inducing errors at midlatitude conditions of up to 15 % above 100 km (20 % for polar summer) and of ∼ 5 % around 80 km. The errors due to uncertainties in the O(1D) and O(3P) profiles are within 3–4 % in the 100–120 km region, and those due to uncertainties in the gain calibration and in the near-infrared solar flux are within ∼ 2 % at all altitudes. The retrieved CO2 shows the major features expected and predicted by general circulation models. In particular, its abrupt decline above 80–90 km and the seasonal change of the latitudinal distribution, with higher CO2 abundances in polar summer from 70 up to ∼ 95 km and lower CO2 vmr in the polar winter. Above ∼ 95 km, CO2 is more abundant in the polar winter than at the midlatitudes and polar summer regions, caused by the reversal of the mean circulation in that altitude region. Also, the solstice seasonal distribution, with a significant pole-to-pole CO2 gradient, lasts about 2.5 months in each hemisphere, while the seasonal transition occurs quickly.

Retrievals of heavy ozone with MIPAS

Abstract. A method for retrieval of 18O-substituted isotopomers of O3 in the stratosphere with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is presented. Using a smoothing regularisation constraint, volume mixing ratio profiles are retrieved for the main isotopologue and the symmetric and asymmetric isotopomers of singly substituted O3. For the retrieval of the heavy isotopologues, two microwindows in the MIPAS A band (685–970 cm−1) and six in the AB band (1020–1170 cm−1) are used. As the retrievals are performed as perturbations on the previously retrieved a priori profiles, the vertical resolution of the individual isotopomer profiles is very similar, which is important when calculating the ratio between two isotopomers. The performance of the method is evaluated using 1044 vertical profiles recorded with MIPAS on 1 July 2003. The mean values are separated by latitude bands, along with estimates of their uncertainties. The asymmetric isotopomer shows a mean enrichment of ∼ 8 %, with a vertical profile that increases up to 33 km and decreases at higher altitudes. This decrease with altitude is a robust result that does not depend on retrieval settings, and it has not been reported clearly in previously published datasets. The symmetric isotopomer is considerably less enriched, with mean values around 3 % and with a large spread. In individual retrievals the uncertainty of the enrichment is dominated by the measurement noise (2–4 %), which can be reduced by averaging multiple retrievals; systematic uncertainties linked to the retrieval are generally small at ∼ 0.5 %, but this is likely underestimated because the uncertainties in key spectroscopic parameters are unknown. The variabilities in the retrieval results are largest for the Southern Hemisphere.

Harmonisation and diagnostics of MIPAS ESA CH<sub>4</sub> and N<sub>2</sub>O profiles using data assimilation

Abstract. This paper discusses assimilation experiments of methane (CH4) and nitrous oxide (N2O) profiles retrieved from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). Here we focus on data versions 6 and 7 provided by the ESA processor. These data sets have been assimilated by the Belgian Assimilation System for Chemical ObsErvations (BASCOE). The CH4 and N2O retrieved profiles can oscillate, especially in the tropical lower stratosphere. Using the averaging kernels of the observations and a background error covariance matrix, which has previously been calibrated, allows the system to partly remedy this issue and provide assimilated fields that are more regular vertically. In general, there is a good agreement between the BASCOE analyses and independent observations from ACE–FTS (CH4 and N2O) and MLS (N2O), demonstrating the general good quality of CH4 and N2O retrievals provided by MIPAS ESA. Nevertheless, this study also identifies two issues in these data sets. First, time series of the observations show unexpected discontinuities due to an abrupt change in the gain of MIPAS band B, generally occurring after the instrument decontamination. Since the calibration is performed weekly, the abrupt change in the gain affects the measurements until the subsequent calibration is performed. Second, the correlations between BASCOE analyses and independent observations are poor in the lower stratosphere, especially in the tropics, probably due to the presence of outliers in the assimilated data. In this region, we recommend using MIPAS CH4 and N2O retrievals with caution.

Direct inversion of circulation and mixing from tracer measurements – Part 1: Method

Abstract. From a series of zonal mean global stratospheric tracer measurements sampled in altitude vs. latitude, circulation and mixing patterns are inferred by the inverse solution of the continuity equation. As a first step, the continuity equation is written as a tendency equation, which is numerically integrated over time to predict a later atmospheric state, i.e., mixing ratio and air density. The integration is formally performed by the multiplication of the initially measured atmospheric state vector by a linear prediction operator. Further, the derivative of the predicted atmospheric state with respect to the wind vector components and mixing coefficients is used to find the most likely wind vector components and mixing coefficients which minimize the residual between the predicted atmospheric state and the later measurement of the atmospheric state. Unless multiple tracers are used, this inversion problem is under-determined, and dispersive behavior of the prediction further destabilizes the inversion. Both these problems are addressed by regularization. For this purpose, a first-order smoothness constraint has been chosen. The usefulness of this method is demonstrated by application to various tracer measurements recorded with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). This method aims at a diagnosis of the Brewer–Dobson circulation without involving the concept of the mean age of stratospheric air, and related problems like the stratospheric tape recorder, or intrusions of mesospheric air into the stratosphere.

Errors induced by different approximations in handling horizontal atmospheric inhomogeneities in MIPAS/ENVISAT retrievals

Abstract. MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) is a mid-infrared limb emission sounder that operated on board the polar satellite ENVISAT from 2002 to 2012. The retrieval algorithm used by the European Space Agency to process MIPAS measurements exploits the assumption that the atmosphere is horizontally homogeneous. However, previous studies highlighted how this assumption causes significant errors on the retrieved profiles of some MIPAS target species.In this paper we quantify the errors induced by this assumption and evaluate the performances of three different algorithms that can be used to mitigate the problem. We generate synthetic observations with a high spatial resolution atmospheric model and carry out the retrievals with four alternative methods. The first assumes horizontal homogeneity (1-D retrieval), the second includes a model of the horizontal gradient of atmospheric temperature (1-D plus temperature gradient retrieval), the third accounts for an horizontal gradient of temperature and composition (1-D plus temperature and composition gradient retrieval), while the fourth is the full two-dimensional (2-D) inversion approach.Our results highlight that the 1-D retrieval implies errors that are significant for averages of profiles. Furthermore, for some targets (e.g. T, CH4 and N2O below 10 hPa) the error induced by the 1-D approximation also becomes visible in the individual retrieved profiles. The inclusion of any kind of horizontal variability model improves all the targets with respect to the horizontal homogeneity assumption. For temperature, HNO3 and CFC-11, the inclusion of an horizontal temperature gradient leads to a significant reduction of the error. For other targets, such as H2O, O3, N2O, CH4, the improvements due to the inclusion of an horizontal temperature gradient are minor. In these cases, the inclusion of a gradient in the target volume mixing ratio leads to significant improvements. Among all the methods tested in this work, the 2-D approach, as expected, implies the smallest errors for almost all the target parameters. This residual error of the 2-D approach is the smoothing caused by the retrieval grid, which is coarser than that of the atmospheric model.

First detection of ammonia (NH<sub>3</sub>) in the Asian summer monsoon upper troposphere

Abstract. Ammonia (NH3) has been detected in the upper troposphere by the analysis of averaged MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) infrared limb-emission spectra. We have found enhanced amounts of NH3 within the region of the Asian summer monsoon at 12–15 km altitude. Three-monthly, 10° longitude × 10° latitude average profiles reaching maximum mixing ratios of around 30 pptv in this altitude range have been retrieved, with a vertical resolution of 3–8 km and estimated errors of about 5 pptv. These observations show that loss processes during transport from the boundary layer to the upper troposphere within the Asian monsoon do not deplete the air entirely of NH3. Thus, ammonia might contribute to the so-called Asian tropopause aerosol layer by the formation of ammonium aerosol particles. On a global scale, outside the monsoon area and during different seasons, we could not detect enhanced values of NH3 above the actual detection limit of about 3–5 pptv. This upper bound helps to constrain global model simulations.

Version 1.3 AIM SOFIE measured methane (CH4): Validation and seasonal climatology

AbstractThe V1.3 methane (CH4) measured by the Aeronomy of Ice in the Mesosphere (AIM) Solar Occultation for Ice Experiment (SOFIE) instrument is validated in the vertical range of ~25–70 km. The random error for SOFIE CH4 is ~0.1–1% up to ~50 km and degrades to ~9% at ∼ 70 km. The systematic error remains at ~4% throughout the stratosphere and lower mesosphere. Comparisons with CH4 data taken by the SCISAT Atmospheric Chemistry Experiment‐Fourier Transform Spectrometer (ACE‐FTS) and the Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) show an agreement within ~15% in the altitude range ~30–60 km. Below ~25 km SOFIE CH4 is systematically higher (≥20%), while above ~65 km it is lower by a similar percentage. The sign change from the positive to negative bias occurs between ~55 km and ~60 km (or ~40 km and ~45 km) in the Northern (or Southern) Hemisphere. Methane, H2O, and 2CH4 + H2O yearly differences from their values in 2009 are examined using SOFIE and MIPAS CH4 and the Aura Microwave Limb Sounder (MLS) measured H2O. It is concluded that 2CH4 + H2O is conserved with altitude up to an upper limit between ~35 km and ~50 km depending on the season. In summer this altitude is higher. In the Northern Hemisphere the difference relative to 2009 is the largest in late spring and the established difference prevails throughout summer and fall, suggesting that summer and fall are dynamically quiet. In both hemispheres during winter there are disturbances (with a period of ~1 month) that travel downward throughout the stratosphere with a speed similar to the winter descent.

Intercomparison and evaluation of satellite peroxyacetyl nitrate observations in the upper troposphere–lower stratosphere

Abstract. Peroxyacetyl nitrate (PAN) is an important chemical species in the troposphere as it aids the long-range transport of NOx and subsequent formation of O3 in relatively clean remote regions. Over the past few decades observations from aircraft campaigns and surface sites have been used to better understand the regional distribution of PAN. However, recent measurements made by satellites allow for a global assessment of PAN in the upper troposphere–lower stratosphere (UTLS). In this study, we investigate global PAN distributions from two independent retrieval methodologies, based on measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on board Envisat from the Institute of Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology, and the Department of Physics and Astronomy, University of Leicester (UoL). Retrieving PAN from MIPAS is challenging due to the weak signal in the measurements and contamination from other species. Therefore, we compare the two MIPAS datasets with observations from the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS), in situ aircraft data and the 3-D chemical transport model TOMCAT. MIPAS shows peak UTLS PAN concentrations over the biomass burning regions (e.g. ranging from 150 to > 200 pptv at 150 hPa) and during the summertime Asian monsoon as enhanced convection aids the vertical transport of PAN from the lower atmosphere. At 150 hPa, we find significant differences between the two MIPAS datasets in the tropics, where IMK PAN concentrations are larger by 50–100 pptv. Comparisons between MIPAS and ACE-FTS show better agreement with the UoL MIPAS PAN concentrations at 200 hPa, but with mixed results above this altitude. TOMCAT generally captures the magnitude and structure of climatological aircraft PAN profiles within the observational variability allowing it to be used to investigate the MIPAS PAN differences. TOMCAT–MIPAS comparisons show that the model is both positively (UoL) and negatively (IMK) biased against the satellite products. These results indicate that satellite PAN observations are able to detect realistic spatial variations in PAN in the UTLS, but further work is needed to resolve differences in existing retrievals to allow quantitative use of the products.

Evaluation of column-averaged methane in models and TCCON with a focus on the stratosphere

Abstract. The distribution of methane (CH4) in the stratosphere can be a major driver of spatial variability in the dry-air column-averaged CH4 mixing ratio (XCH4), which is being measured increasingly for the assessment of CH4 surface emissions. Chemistry-transport models (CTMs) therefore need to simulate the tropospheric and stratospheric fractional columns of XCH4 accurately for estimating surface emissions from XCH4. Simulations from three CTMs are tested against XCH4 observations from the Total Carbon Column Network (TCCON). We analyze how the model–TCCON agreement in XCH4 depends on the model representation of stratospheric CH4 distributions. Model equivalents of TCCON XCH4 are computed with stratospheric CH4 fields from both the model simulations and from satellite-based CH4 distributions from MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) and MIPAS CH4 fields adjusted to ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. Using MIPAS-based stratospheric CH4 fields in place of model simulations improves the model–TCCON XCH4 agreement for all models. For the Atmospheric Chemistry Transport Model (ACTM) the average XCH4 bias is significantly reduced from 38.1 to 13.7 ppb, whereas small improvements are found for the models TM5 (Transport Model, version 5; from 8.7 to 4.3 ppb) and LMDz (Laboratoire de Météorologie Dynamique model with zooming capability; from 6.8 to 4.3 ppb). Replacing model simulations with MIPAS stratospheric CH4 fields adjusted to ACE-FTS reduces the average XCH4 bias for ACTM (3.3 ppb), but increases the average XCH4 bias for TM5 (10.8 ppb) and LMDz (20.0 ppb). These findings imply that model errors in simulating stratospheric CH4 contribute to model biases. Current satellite instruments cannot definitively measure stratospheric CH4 to sufficient accuracy to eliminate these biases. Applying transport diagnostics to the models indicates that model-to-model differences in the simulation of stratospheric transport, notably the age of stratospheric air, can largely explain the inter-model spread in stratospheric CH4 and, hence, its contribution to XCH4. Therefore, it would be worthwhile to analyze how individual model components (e.g., physical parameterization, meteorological data sets, model horizontal/vertical resolution) impact the simulation of stratospheric CH4 and XCH4.

Phosgene in the UTLS: seasonal and latitudinal variations from MIPAS observations

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is a Fourier transform spectrometer that measured mid-infrared atmospheric limb emission spectra from July 2002 to April 2012 on board the polar-orbiting satellite ENVISAT. We have used MIPAS data to study the latitudinal variations of phosgene (COCl2 or carbonyl chloride) and, for the first time, its seasonal variation in the upper troposphere/lower stratosphere region (UTLS). Retrievals of phosgene were made using the 830–860 cm−1 region, corresponding to the ν5 bands of COCl2. Unfortunately, in that region, the ν4 band of CFC-11, which is much stronger than COCl2 ν5, hides the phosgene emission. In order to evaluate seasonality and latitudinal distribution of phosgene we have analysed all the measurements made by MIPAS on days 18 and 20 of each month of 2008 with the optimized retrieval model (ORM) recently upgraded with the multi-target retrieval technique and with the optimal estimation functionality to apply external constraints to the state vector. Average seasonal profiles of phosgene show an evident latitudinal variability with the largest values observed in the tropical regions (maximum ≈ 35 parts per trillion by volume (pptv) at about 300 hPa). In the midlatitude and polar regions, the volume mixing ratio (VMR) values do not exceed 30 pptv and the vertical distributions are less peaked. Our analysis highlights that COCl2 seasonal variability is fairly low, apart from the polar regions.

Infrared limb emission measurements of aerosol in the troposphere and stratosphere

Abstract. Altitude-resolved aerosol detection in the upper troposphere and lower stratosphere (UTLS) is a challenging task for remote sensing instruments. Infrared limb emission measurements provide vertically resolved global measurements at day- and nighttime in the UTLS. For high-spectral-resolution infrared limb instruments we present here a new method to detect aerosol and separate between ice and non-ice particles. The method is based on an improved aerosol–cloud index that identifies infrared limb emission spectra affected by non-ice aerosol or ice clouds. For the discrimination between non-ice aerosol and ice clouds we employed brightness temperature difference correlations. The discrimination thresholds for this method were derived from radiative transfer simulations (including scattering) and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS)/Envisat measurements obtained in 2011. We demonstrate the value of this approach for observations of volcanic ash and sulfate aerosol originating from the Grímsvötn (Iceland, 64° N), Puyehue–Cordón Caulle (Chile, 40° S), and Nabro (Eritrea, 13° N) eruptions in May and June 2011 by comparing the MIPAS volcanic aerosol detections with Atmospheric Infrared Sounder (AIRS) volcanic ash and SO2 measurements.

Evaluation of water vapour assimilation in the tropical upper troposphere and lower stratosphere by a chemical transport model

Abstract. The present analysis deals with one of the most debated aspects of the studies on the upper troposphere/lower stratosphere (UTLS), namely the budget of water vapour (H2O) at the tropical tropopause. Within the French project “Multiscale water budget in the upper troposphere and lower stratosphere in the TROpics” (TRO-pico), a global-scale analysis has been set up based on space-borne observations, models and assimilation techniques. The MOCAGE-VALENTINA assimilation tool has been used to assimilate the Aura Microwave Limb Sounder (MLS) version 3.3 H2O measurements within the 316–5 hPa range from August 2011 to March 2013 with an assimilation window of 1 h. Diagnostics based on observations minus analysis and forecast are developed to assess the quality of the assimilated H2O fields. Comparison with an independent source of H2O measurements in the UTLS based on the space-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observations and with meteorological ARPEGE analyses is also shown. Sensitivity studies of the analysed fields have been performed by (1) considering periods when no MLS measurements are available and (2) using H2O data from another MLS version (4.2). The studies have been performed within three different spaces in time and space coincidences with MLS (hereafter referred to as MLS space) and MIPAS (MIPAS space) observations and with the model (model space) outputs and at three different levels: 121 hPa (upper troposphere), 100 hPa (tropopause) and 68 hPa (lower stratosphere) in January and February 2012. In the MLS space, the analyses behave consistently with the MLS observations from the upper troposphere to the lower stratosphere. In the model space, the analyses are wetter than the reference atmosphere as represented by ARPEGE and MLS in the upper troposphere (121 hPa) and around the tropopause (100 hPa), but are consistent with MLS and MIPAS in the lower stratosphere (68 hPa). In the MIPAS space, the sensitivity and the vertical resolution of the MIPAS data set at 121 and 100 hPa prevent assessment of the behaviour of the analyses at 121 and 100 hPa, particularly over intense convective areas as the South American, the African and the Maritime continents but, in the lower stratosphere (68 hPa), the analyses are very consistent with MIPAS. Sensitivity studies show the improvement on the H2O analyses in the tropical UTLS when assimilating space-borne measurements of better quality, particularly over the convective areas.

A multi-wavelength classification method for polar stratospheric cloud types using infrared limb spectra

Abstract. The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on board the ESA Envisat satellite operated from July 2002 until April 2012. The infrared limb emission measurements represent a unique dataset of daytime and night-time observations of polar stratospheric clouds (PSCs) up to both poles. Cloud detection sensitivity is comparable to space-borne lidars, and it is possible to classify different cloud types from the spectral measurements in different atmospheric windows regions. Here we present a new infrared PSC classification scheme based on the combination of a well-established two-colour ratio method and multiple 2-D brightness temperature difference probability density functions. The method is a simple probabilistic classifier based on Bayes' theorem with a strong independence assumption. The method has been tested in conjunction with a database of radiative transfer model calculations of realistic PSC particle size distributions, geometries, and composition. The Bayesian classifier distinguishes between solid particles of ice and nitric acid trihydrate (NAT), as well as liquid droplets of super-cooled ternary solution (STS). The classification results are compared to coincident measurements from the space-borne lidar Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument over the temporal overlap of both satellite missions (June 2006–March 2012). Both datasets show a good agreement for the specific PSC classes, although the viewing geometries and the vertical and horizontal resolution are quite different. Discrepancies are observed between the CALIOP and the MIPAS ice class. The Bayesian classifier for MIPAS identifies substantially more ice clouds in the Southern Hemisphere polar vortex than CALIOP. This disagreement is attributed in part to the difference in the sensitivity on mixed-type clouds. Ice seems to dominate the spectral behaviour in the limb infrared spectra and may cause an overestimation in ice occurrence compared to the real fraction of ice within the PSC area in the polar vortex. The entire MIPAS measurement period was processed with the new classification approach. Examples like the detection of the Antarctic NAT belt during early winter, and its possible link to mountain wave events over the Antarctic Peninsula, which are observed by the Atmospheric Infrared Sounder (AIRS) instrument, highlight the importance of a climatology of 9 Southern Hemisphere and 10 Northern Hemisphere winters in total. The new dataset is valuable both for detailed process studies, and for comparisons with and improvements of the PSC parameterizations used in chemistry transport and climate models.