ALBERT

Description: We report on HCFC-22 data acquired by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) in the reduced spectral resolution nominal observation mode. The data cover the period from January 2005 to April 2012 and the altitude range from the upper troposphere (above cloud top altitude) to about 50 km. The profile retrieval was performed by constrained nonlinear least squares fitting of modelled spectra to the measured limb spectral radiances. The spectral ν4-band at 816.5 ± 13 cm−1 was used for the retrieval. A Tikhonov-type smoothing constraint was applied to stabilise the retrieval. In the lower stratosphere, we find a global volume mixing ratio of HCFC-22 of about 185 pptv in January 2005. The rate of linear growth in the lower latitudes lower stratosphere was about 6 to 7 pptv year−1 in the period 2005–2012. The profiles obtained were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon profiles and cryosampler balloon measurements. Between 13 and 22 km, average agreement within −3 to +5 pptv (MIPAS – ACE) with ACE-FTS v3.5 profiles is demonstrated. Agreement with MkIV solar occultation balloon-borne measurements is within 10–20 pptv below 30 km and worse above, while in situ cryosampler balloon measurements are systematically lower over their full altitude range by 15–50 pptv below 24 km and less than 10 pptv above 28 km. MIPAS HCFC-22 time series below 10 km altitude are shown to agree mostly well to corresponding time series of near-surface abundances from the NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is obvious in the satellite data. This is attributed to tropopause altitude fluctuations and subsidence of polar winter stratospheric air into the troposphere. A parametric model consisting of constant, linear, quasi-biennial oscillation (QBO) and several sine and cosine terms with different periods has been fitted to the temporal variation of stratospheric HCFC-22 for all 10°-latitude/1-to-2-km-altitude bins. The relative linear variation was always positive, with relative increases of 40–70 % decade−1 in the tropics and global lower stratosphere, and up to 120 % decade−1 in the upper stratosphere of the northern polar region and the southern extratropical hemisphere. Asian HCFC-22 emissions have become the major source of global upper tropospheric HCFC-22. In the upper troposphere, monsoon air, rich in HCFC-22, is instantaneously mixed into the tropics. In the middle stratosphere, between 20 and 30 km, the observed trend is inconsistent with the trend at the surface (corrected for the age of stratospheric air), hinting at circulation changes. There exists a stronger positive trend in HCFC-22 in the Southern Hemisphere and a more muted positive trend in the Northern Hemisphere, implying a potential change in the stratospheric circulation over the observation period.

Description: 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. As 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.

Description: Vertically resolved distributions of sulfur dioxide (SO2) with global coverage in the height region from the upper troposphere to ~ 20 km altitude have been derived from observations by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat for the period July 2002 to April 2012. Retrieved volume mixing ratio profiles representing single measurements are characterized by typical errors in the range of 70–100 pptv and by a vertical resolution ranging from 3–5 km. Comparison with ACE-FTS observations revealed a slightly varying bias with altitude of −20 to 50 pptv for the MIPAS dataset in case of volcanically enhanced concentrations. For background concentrations the comparison showed a systematic difference between the two major MIPAS observation periods. After debiasing, the difference could be reduced to biases within −10 to 20 pptv in the altitude range of 10–20 km with respect to ACE-FTS. Further comparisons of the debiased MIPAS dataset with in-situ measurements from various aircraft campaigns showed no obvious inconsistencies within a range of around ±50 pptv. The SO2 emissions of more than thirty volcanic eruptions could be identified in the upper troposphere and lower stratosphere (UTLS). Emitted SO2 masses and lifetimes within different altitude ranges in the UTLS have been derived for a large part of these eruptions. Masses are in most cases within estimations derived from other instruments. From three of the major eruptions within the MIPAS measurement period – Kasatochi in August 2008, Sarychev in June 2009 and Nabro in June 2011 – derived lifetimes of SO2 for the altitude ranges 10–14, 14–18, and 18–22 km are 13.3±2.1, 23.6±1.2, and 32.3±5.5 d, respectively. By omitting periods with obvious volcanic influence we have derived background mixing ratio distributions of SO2. At 10 km altitude these indicate an annual cycle at northern mid- and high latitudes with maximum values in summer and an amplitude of about 30 pptv. At higher altitudes of about 16–18 km enhanced mixing ratios of SO2 can be found in the region of the Asian and the North-American monsoon in summer – a possible connection to an aerosol layer discovered by Vernier et al. (2011b) in that region.

Description: 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), insitu aircraft data and the TOMCAT 3-D chemical transport model. 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 show 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.

Description: We report on HCFC-22 data acquired by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) in reduced spectral resolution nominal mode in the period from January 2005 to April 2012 from version 5.02 level-1b spectral data and covering an altitude range from the upper troposphere (above cloud top altitude) to about 50 km. The profile retrieval was performed by constrained nonlinear least squares fitting of measured limb spectral radiances to modelled spectra. The spectral ν4-band at 816.5 ± 13 cm−1 was used for the retrieval. A Tikhonov-type smoothing constraint was applied to stabilise the retrieval. In the lower stratosphere, we find a global volume mixing ratio of HCFC-22 of about 185 pptv in January 2005. The linear growth rate in the lower latitudes lower stratosphere was about 6 to 7 pptv yr−1 in the period 2005–2012. The obtained profiles were compared with ACE-FTS satellite data v3.5, as well as with MkIV balloon profiles and in situ cryosampler balloon measurements. Between 13 and 22 km, average agreement within −3 to +5 pptv (MIPAS–ACE) with ACE-FTS v3.5 profiles is demonstrated. Agreement with MkIV solar occultation balloon-borne measurements is within 10–20 pptv below 30 km and worse above, while in situ cryosampler balloon measurements are systematically lower over their full altitude range by 15–50 pptv below 24 km and less than 10 pptv above 28 km. Obtained MIPAS HCFC-22 time series below 10 km altitude are shown to agree mostly well to corresponding time series of near-surface abundances from NOAA/ESRL and AGAGE networks, although a more pronounced seasonal cycle is obvious in the satellite data, probably due to tropopause altitude fluctuations and subsidence of polar winter stratospheric air into the troposphere. A parametric model consisting of constant, linear, quasi-biennial oscillation (QBO) and several sine and cosine terms with different periods has been fitted to the temporal variation of stratospheric HCFC-22 for all 10° latitude/1 to 2 km altitude bins. The relative linear variation was always positive, with relative increases of 40–70% decade−1 in the tropics and global lower stratosphere, and up to 120% decade−1 in the upper stratosphere of the northern polar region and the southern extratropical hemisphere. In the middle stratosphere between 20 and 30 km, the observed trend is not consistent with the age of stratospheric air-corrected trend at ground, but stronger positive at the Southern Hemisphere and less strong increasing in the Northern Hemisphere, hinting towards changes in the stratospheric circulation over the observation period.

Description: A new and improved setup of the SF6 retrieval together with a newly calibrated version of MIPAS-ENVISAT level 1b spectra (version 5, ESA data version 5.02/5.06) was used to obtain a new global SF6-data set, covering the total observational period of MIPAS from July 2002 to April 2012 for the first time. Monthly and zonally averaged SF6-profiles were converted into mean age of air using a tropospheric SF6-reference curve. The obtained data set of age of air was compared to airborne and balloon-borne age of air measurements. The temporal evolution of mean age of air was then investigated in 10° latitude and 1–2 km altitude bins. A regression model consisting of a constant and a linear trend term, 2 proxies for the quasi-biennial oscillation variation, sinusoidal terms for the seasonal and semi-annual variation and overtones was fitted to the age of air time series. The annual cycle for particular regions in the stratosphere was investigated and compared to other studies. The age of air trend over the total MIPAS-period consisting of the linear term was assessed and compared to previous findings of Stiller et al. (2012). While the linear increase of mean age is confirmed to be positive for the Northern mid-latitudes and Southern polar middle stratosphere, differences are found in the Northern polar upper stratosphere, where the mean age is now found to increase as well. The magnitude of trends in the Northern mid-latitude middle stratosphere is slightly lower compared to the previous version and the trends fit remarkably well to the trend derived by Engel et al. (2009). Negative age of air trends found by Stiller et al. (2012) are confirmed for the lowermost tropical stratosphere and lowermost Southern mid-latitudinal stratosphere. Differences to the previous data versions occur in the middle tropical stratosphere around 25 km, where the trends are now negative. Overall, the new latitude–altitude distribution of trends appears to be less patchy and more coherent than the previous one. The new data provide evidence of an accelerating shallow branch of the Brewer–Dobson circulation, at least in the Southern Hemisphere. Finally the age of air decadal trends are compared to trends calculated with simulated SF6 values by the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) and good agreement is found. The hemispheric asymmetry in the trends found in the MIPAS data are also indicated in the trends calculated with simulated SF6 values by the KASIMA model.

Description: We present the strongly revised IMK/IAA MIPAS-ENVISAT CH4 and N2O data products for the MIPAS full-resolution (versions V5H_CH4_21 and V5H_N2O_21) and for the reduced-resolution period (versions V5R_CH4_224, V5R_CH4_225, V5R_N2O_224 and V5R_N2O_225). These data sets cover both MIPAS measurement periods from June 2002 until March 2004 and from January 2005 to April 2012. Differences with older retrieval versions which are known to have a high bias are discussed. The usage of the HITRAN 2008 spectroscopic data set leads to lower values for both gases in the lower part of the profile. The improved correction of additive radiance offsets and handling of background radiance continua allows for aerosol contributions at altitudes in the upper stratosphere and above. These changes lead to more plausible values, both in the radiance offset and in the profiles of the continuum absorption coefficients. They also increase the fraction of converged retrievals. Some minor changes were applied to the constraint of the inverse problem, causing small differences in the retrieved profiles, mostly due to the relaxation of off-diagonal regularisation matrix elements for the calculation of jointly retrieved absorption coefficient profiles. Spectral microwindows have been adjusted to avoid areas with saturated spectral signatures. Jointly retrieving profiles of water vapour and nitric acid serves to compensate spectroscopic inconsistencies. We discuss the averaging kernels of the profiles and their vertical resolution. The latter ranges from 2.5 to 7 km for CH4, and from 2.5 to 6 km for N2O in the reduced-resolution period. For the full-resolution period, the vertical resolution is in the order of 3 to 6 km for both gases. We find the retrieval errors in the lower part of the profiles mostly to be around 15 % for CH4 and below 10 % for N2O. The errors above 25 or 30 km increase to values between 10 and 20 %, except for CH4 from the reduced-resolution period, where the estimated errors stay below 15 %.

Description: The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) is an infrared (IR) limb emission spectrometer on the Envisat platform. It measures trace gas distributions during day and night, pole-to-pole, over an altitude range from 6 to 70 km in nominal mode and up to 170 km in special modes, depending on the measurement mode, producing more than 1000 profiles day−1. We present the results of a validation study of methane, version V5R_CH4_222, retrieved with the IMK/IAA (Institut für Meteorologie und Klimaforschung, Karlsruhe/Instituto de Astrofisica de Andalucia, Grenada) MIPAS scientific level 2 processor. The level 1 spectra are provided by the ESA (European Space Agency) and version 5 was used. The time period covered is 2005–2012, which corresponds to the period when MIPAS measured trace gas distributions at a reduced spectral resolution of 0.0625 cm−1. The comparison with satellite instruments includes the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the HALogen Occultation Experiment (HALOE), the Solar Occultation For Ice Experiment (SOFIE) and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). Furthermore, comparisons with MkIV balloon-borne solar occultation measurements and with air sampling measurements performed by the University of Frankfurt are presented. The validation activities include bias determination, assessment of stability, precision validation, analysis of histograms and comparison of corresponding climatologies. Above 50 km altitude, MIPAS methane mixing ratios agree within 3 % with ACE-FTS and SOFIE. Between 30 and 40 km an agreement within 3 % with SCIAMACHY has been found. In the middle stratosphere, there is no clear indication of a MIPAS bias since comparisons with various instruments contradict each other. In the lower stratosphere (below 25 km) MIPAS CH4 is biased high with respect to satellite instruments, and the most likely estimate of this bias is 14 %. However, in the comparison with CH4 data obtained from cryogenic whole-air sampler (cryosampler) measurements, there is no evidence of a high bias in MIPAS between 20 and 25 km altitude. Precision validation is performed on collocated MIPAS–MIPAS pairs and suggests a slight underestimation of its uncertainties by a factor of 1.2. No significant evidence of an instrumental drift has been found.

Description: 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 MIPAS/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 Científicas (CSIC), Instituto de Astrofísica de Andalucía (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  ∼  15 and 30 km, most comparisons agree within 10–20 pptv (10–20 %), apart from ILAS-II, which shows large differences above  ∼  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  ∼  30 km. Above that altitude, larger drifts of up to  ∼  50 % decade−1 appear which are negative up to  ∼  35 km and positive, but of a similar magnitude, above.