Maximum likelihood representation of MIPAS profiles

In order to avoid problems connected with the content of a priori information in volume mixing ratio vertical profiles measured with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), a user-friendly representation of the data has been developed which will be made available in addition to the regular data product. In this representation, the data will be provided on a fixed pressure grid coarse enough to allow a virtually unconstrained retrieval. To avoid data interpolation, the grid is chosen to be a subset of the pressure grids used by the Chemistry-Climate Model Initiative and the Data Initiative within the Stratosphere-troposphere Processes And their Role in Climate (SPARC) project as well as the Intergovernmental Panel of Climate Change climatologies and model calculations. For representation, the profiles have been transformed to boxcar base functions, which means that volume mixing ratios are constant within a layer. This representation is thought to be more adequate for comparison with model data. While this method is applicable also to vertical profiles of other species, the method is discussed using ozone as an example

Retrievals of heavy ozone with MIPAS

A method for retrieval of $^{18}$O-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

Observed temporal evolution of global mean age of stratospheric air for the 2002 to 2010 period

An extensive observational data set, consisting of more than 106 SF6 vertical profiles distributed globally from MIPAS measurements has been condensed into monthly zonal means of mean age of air for the period September 2002 to January 2010, binned at 10$^\circ$ latitude and 1–2 km altitude. The data were analysed with respect to their temporal variation by fitting a regression model consisting of a constant and a linear increase term, 2 proxies for the QBO variation, sinusoidal terms for the seasonal and semiannual variation and overtones for the correction of the shapes to the observed data set. The impact of subsidence of mesospheric SF6-depleted air and in-mixing into non-polar latitudes on mid-latitudinal absolute age of air and its linear increase was assessed and found to be small. The linear increase of mean age of stratospheric air was found to be positive and partly larger than the trend derived by Engel et al. (2009) for most of the Northern mid-latitudes, the middle stratosphere in the tropics, and parts of the Southern mid latitudes, as well as for the Southern polar upper stratosphere. Multi-year decrease of age of air was found for the lowermost and the upper stratospheric tropics, for parts of Southern mid-latitudes, and for the Northern polar regions. Analysis of the amplitudes and phases of the seasonal variation shed light on the coupling of stratospheric regions to each other. In particular, the Northern mid-latitude stratosphere is well coupled to the tropics, while the Northern lowermost mid-latitudinal stratosphere is decoupled, confirming the separation of the shallow branch of the Brewer-Dobson circulation from the deep branch. We suggest an overall increased tropical upwelling, together with weakening of mixing barriers, especially in the Northern Hemisphere, as a hypothetical model to explain the observed pattern of linear multi-year increase/decrease, and amplitudes and phase shifts of the seasonal variation

Carbon monoxide distributions from the upper troposphere to the mesosphere inferred from 4.7 μm non-local thermal equilibrium emissions measured by MIPAS on Envisat

We present global distributions of carbon monoxide (CO) from the upper troposphere to the mesosphere observed by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat. Vertically resolved volume mixing ratio profiles have been retrieved from 4.7 μm limb emission spectra under consideration of non-local thermodynamic equilibrium. The precision of individual CO profiles is typically 5–30 ppbv (15–40% for altitudes greater than 40 km and lower than 15 km and 30–90% within 15–40 km). Estimated systematic errors are in the order of 8–15%. Below 60 km, the vertical resolution is 4–7 km. The data set which covers 54 days from September 2003 to March 2004 has been derived with an improved retrieval version including (i) the retrieval of log(vmr), (ii) the consideration of illumination-dependent vibrational population gradients along the instrument's line of sight, and (iii) joint-fitted vmr horizontal gradients in latitudinal and longitudinal directions. A detailed analysis of spatially resolved CO distributions during the 2003/2004 Northern Hemisphere major warming event demonstrate the potential of MIPAS CO observations to obtain new information on transport processes during dynamical active episodes, particularly on those acting in the vertical. From the temporal evolution of zonally averaged CO abundances, we derived extraordinary polar winter descent velocities of 1200 m per day inside the recovered polar vortex in January 2004. Middle stratospheric CO abundances show a well established correlation with the chemical source CH<sub>4</sub>, particularly in the tropics. In the upper troposphere, a moderate CO decrease from September 2003 to March 2004 was observed. Upper tropospheric CO observations provide a detailed picture of long-range transport of polluted air masses and uplift events. MIPAS observations taken on 9–11 September 2003 confirm the trapping of convective outflow of polluted CO-rich air from Southeast Asia into the Asian monsoon anticyclone, which has been described in previous studies. Upper tropospheric CO plumes, observed by MIPAS on this day, were predominantly located in the Northern Hemisphere. Most of these plumes could be related to Southeast Asian pollution by means of backward trajectory calculations. During 20–22 October, southern hemispheric biomass burning was the most likely source of the major CO plumes observed over the Southern Atlantic and Indian Ocean

MIPAS IMK/IAA CFC-11 (CCl3F) and CFC-12 (CCl2F2) Measurements: Accuracy, Precision and Long-Term Stability

Profiles of CFC-11 (CCl3F) and CFC-12 (CCl2F2) of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European satellite Envisat have been retrieved from versions MIPAS/4.61 to MI-PAS/4.62 and MIPAS/5.02 to MIPAS/5.06 level-1b data using the scientific level-2 processor run by Karlsruhe Institute of Technology (KIT), Institute of Meteorology and Climate Research (IMK) and Consejo Superior de Investigaciones Cientificas (CSIC), Instituto de Astrofisica de Andalucia (IAA). These profiles have been compared to measurements taken by the balloon-borne cryosampler, Mark IV (MkIV) and MIPAS-Balloon (MIPAS-B), the airborne MIPAS-STRatospheric aircraft (MIPAS-STR), the satellite-borne Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) and the High Resolution Dynamic Limb Sounder (HIRDLS), as well as the ground-based Halocarbon and other Atmospheric Trace Species (HATS) network for the reduced spectral resolution period (RR: January 2005-April 2012) of MIPAS. ACE-FTS, MkIV and HATS also provide measurements during the high spectral resolution period (full resolution, FR: July 2002-March 2004) and were used to validate MIPAS CFC-11 and CFC-12 products during that time, as well as profiles from the Improved Limb Atmospheric Spectrometer, ILAS-II. In general, we find that MIPAS shows slightly higher values for CFC-11 at the lower end of the profiles (below ~ 15 km) and in a comparison of HATS ground-based data and MIPAS measurements at 3 km below the tropopause. Differences range from approximately 10 to 50 pptv (~ 5-20 %) during the RR period. In general, differences are slightly smaller for the FR period. An indication of a slight high bias at the lower end of the profile exists for CFC-12 as well, but this bias is far less pronounced than for CFC-11 and is not as obvious in the relative differences between MIPAS and any of the comparison instruments. Differences at the lower end of the profile (below ~15 km) and in the comparison of HATS and MIPAS measurements taken at 3 km below the tropopause mainly stay within 10-50 pptv (corresponding to ~ 2-10% for CFC-12) for the RR and the FR period. Between similar to 15 and 30 km, most comparisons agree within 10-20 pptv (10-20 %), apart from ILAS-II, which shows large differences above similar to 17 km. Overall, relative differences are usually smaller for CFC-12 than for CFC-11. For both species -CFC-11 and CFC-12 - we find that differences at the lower end of the profile tend to be larger at higher latitudes than in tropical and subtropical regions. In addition, MIPAS profiles have a maximum in their mixing ratio around the tropopause, which is most obvious in tropical mean profiles. Comparisons of the standard deviation in a quiescent atmosphere (polar summer) show that only the CFC-12 FR error budget can fully explain the observed variability, while for the other products (CFC-11 FR and RR and CFC-12 RR) only two-thirds to three-quarters can be explained. Investigations regarding the temporal stability show very small negative drifts in MIPAS CFC-11 measurements. These instrument drifts vary between ~ 1 and 3% decade-1. For CFC-12, the drifts are also negative and close to zero up to similar to 30 km. Above that altitude, larger drifts of up to similar to 50% decade-1 appear which are negative up to similar to 35 km and positive, but of a similar magnitude, above

HOCl chemistry in the Antarctic stratospheric vortex 2002, as observed with the Michelson interferometer for passive atmospheric sounding (MIPAS)

In the 2002 Antarctic polar vortex enhanced HOCl mixing ratios were detected by the Michelson Interferometer for Passive Atmospheric Sounding both at altitudes of around 35 km (1000K potential temperature), where HOCl abundances are ruled by gas phase chemistry and at around 18–24 km (475–625 K), which belongs to the altitude domain where heterogeneous chlorine chemistry is relevant. At altitudes of 33 to 40 km polar vortex HOCl mixing ratios were found to be around 0.14 ppbv as long as the polar vortex was intact, centered at the pole, and thus received relatively little sunlight. This is the altitude region where in midlatitudinal and tropic atmospheres peak HOCl mixing ratios significantly above 0.2 ppbv (in terms of daily mean values) are observed. After deformation and displacement of the polar vortex in the course of a major warming, ClO-rich vortex air was more exposed to sunlight, where enhanced HOx abundances led to largely increased HOCl mixing ratios (up to 0.3 ppbv), exceeding typical midlatitudinal and tropical amounts significantly. The HOCl increase was preceded by an increase of ClO. Model runs could reproduce these measurements only when the Stimpfle et al. (1979) rate constant for the reaction ClO+HO2→HOCl+O2 was used but not with the current JPL recommendation. At an altitude of 24 km, HOCl mixing ratios of up to 0.15 ppbv were detected. This HOCl enhancement, which is already visible in 18 September data, is attributed to heterogeneous chemistry, which is in agreement with observations of polar stratospheric clouds. The measurements were compared to a model run where no polar stratospheric clouds appeared during the observation period. The fact that HOCl still was produced in the model run suggests that a significant part of HOCl was generated from ClO rather than directly via heterogeneous reaction. Excess ClO, lower ClONO2 and earlier loss of HOCl in the measurements are attributed to ongoing heterogeneous chemistry which is not reproduced by the model. On 11 October, polar vortex mean daytime mixing ratios were only 0.03 ppbv

Retrieval of temperature, H₂O, O₃, HNO₃, CH₄, N₂O, ClONO₂ and ClO from MIPAS reduced resolution nominal mode limb emission measurements

Retrievals of temperature, H2O, O3, HNO3, CH4, N2O, ClONO2 and ClO from MIPAS reduced spectral resolution nominal mode limb emission measurements outperform retrievals from respective full spectral resolution measurements both in terms of altitude resolution and precision. The estimated precision (including measurement noise and propagation of uncertain parameters randomly varying in the time domain) and altitude resolution are typically 0.5–1.4K and 2–3.5 km for temperature between 10 and 50 km altitude, and 5–6%, 2–4 km for H2O below 30 km altitude, 4– 5%, 2.5–4.5 km for O3 between 15 and 40 km altitude, 3– 8%, 3–5 km for HNO3 between 10 and 35 km altitude, 5– 8%, 2–3 km for CH4 between 15 and 35 km altitude, 5–10%, 3 km for N2O between 15 and 35 km altitude, 8–14%, 2.5– 9 km for ClONO2 below 40 km, and larger than 35%, 3– 7 km for ClO in the lower stratosphere. As for the full spectral resolution measurements, the reduced spectral resolution nominal mode horizontal sampling (410 km) is coarser than the horizontal smoothing (often below 400 km), depending on species, altitude and number of tangent altitudes actually used for the retrieval. Thus, aliasing might be an issue even in the along-track domain. In order to prevent failure of convergence, it was found to be essential to consider horizontal temperature gradients during the retrieval

Validation of MIPAS IMK/IAA V5R_O3_224 Ozone Profiles

We present the results of an extensive validation program of the most recent version of ozone vertical profiles retrieved with the IMK/IAA (Institute for Meteorology and Climate Research/Instituto de Astrofisica de Andalucia) MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) research level 2 processor from version 5 spectral level 1 data. The time period covered corresponds to the reduced spectral resolution period of the MIPAS instrument, i.e., January 2005-April 2012. The comparison with satellite instruments includes all post-2005 satellite limb and occultation sensors that have measured the vertical profiles of tropospheric and stratospheric ozone: ACE-FTS, GOMOS, HALOE, HIRDLS, MLS, OSIRIS, POAM, SAGE II, SCIAMACHY, SMILES, and SMR. In addition, balloon-borne MkIV solar occultation measurements and ground-based Umkehr measurements have been included, as well as two nadir sensors: IASI and SBUV. For each reference data set, bias determination and precision assessment are performed. Better agreement with reference instruments than for the previous data version, V5R_O3_220 (Laeng et al., 2014), is found: the known high bias around the ozone vmr (volume mixing ratio) peak is significantly reduced and the vertical resolution at 35 km has been improved. The agreement with limb and solar occultation reference instruments that have a known small bias vs. ozonesondes is within 7% in the lower and middle stratosphere and 5% in the upper troposphere. Around the ozone vmr peak, the agreement with most of the satellite reference instruments is within 5 %; this bias is as low as 3% for ACE-FTS, MLS, OSIRIS, POAM and SBUV