ALBERT

Description: The paper presents a comparative study of age of air (AoA) derived from several approaches: a widely used passive-tracer accumulation method, the SF6 accumulation, and a direct calculation of an ideal-age tracer. The simulations were performed with the Eulerian chemistry transport model SILAM driven with the ERA-Interim reanalysis for 1980–2018. The Eulerian environment allowed for simultaneous application of several approaches within the same simulation and interpretation of the obtained differences. A series of sensitivity simulations revealed the role of the vertical profile of turbulent diffusion in the stratosphere, destruction of SF6 in the mesosphere, and the effect of gravitational separation of gases with strongly different molar masses. The simulations reproduced well the main features of the SF6 distribution in the atmosphere observed by the MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) satellite instrument. It was shown that the apparent very old air in the upper stratosphere derived from the SF6 profile observations is a result of destruction and gravitational separation of this gas in the upper stratosphere and the mesosphere. These processes make the apparent SF6 AoA in the stratosphere several years older than the ideal-age AoA, which, according to our calculations, does not exceed 6–6.5 years. The destruction of SF6 and the varying rate of emission make SF6 unsuitable for reliably deriving AoA or its trends. However, observations of SF6 provide a very useful dataset for validation of the stratospheric circulation in a model with the properly implemented SF6 loss.

Description: Remote sensing of atmospheric state variables typically relies on the inverse solution of the radiative transfer equation. An adequately characterized retrieval provides information on the uncertainties of the estimated state variables as well as on how any constraint or a priori assumption affects the estimate. Reported characterization data should be intercomparable between different instruments, empirically validatable, grid-independent, usable without detailed knowledge of the instrument or retrieval technique, traceable and still have reasonable data volume. The latter may force one to work with representative rather than individual characterization data. Many errors derive from approximations and simplifications used in real-world retrieval schemes, which are reviewed in this paper, along with related error estimation schemes. The main sources of uncertainty are measurement noise, calibration errors, simplifications and idealizations in the radiative transfer model and retrieval scheme, auxiliary data errors, and uncertainties in atmospheric or instrumental parameters. Some of these errors affect the result in a random way, while others chiefly cause a bias or are of mixed character. Beyond this, it is of utmost importance to know the influence of any constraint and prior information on the solution. While different instruments or retrieval schemes may require different error estimation schemes, we provide a list of recommendations which should help to unify retrieval error reporting.

Description: A ground-based, high-spectral-resolution Fourier transform infrared (FTIR) spectrometer has been operational in Addis Ababa, Ethiopia (9.01∘ N latitude, 38.76∘ E longitude; 2443 m altitude above sea level), since May 2009 to obtain information on column abundances and profiles of various constituents in the atmosphere. Vertical profile and column abundances of methane and nitrous oxide are derived from solar absorption measurements taken by FTIR for a period that covers May 2009 to March 2013 using the retrieval code PROFFIT (V9.5). A detailed error analysis of CH4 and N2O retrieval are performed. Averaging kernels of the target gases shows that the major contribution to the retrieved information comes from the measurement. Thus, average degrees of freedom for signals are found to be 2.1 and 3.4, from the retrieval of CH4 and N2O for the total observed FTIR spectra. Methane and nitrous oxide volume mixing ratio (VMR) profiles and column amounts retrieved from FTIR spectra are compared with data from the reduced spectral resolution Institute of Meteorology and Climate Research/Instituto de Astrofísica de Andalucía (IMK/IAA) MIPAS (Version V5R_CH4_224 and V5R_N2O_224), the Microwave Limb Sounder (MLS) (MLS v3.3 of N2O and CH4 derived from MLS v3.3 products of CO, N2O, and H2O), and the Atmospheric Infrared Sounder (AIRS) sensors on board satellites. The averaged mean relative difference between FTIR methane and the three correlative instruments MIPAS, MLS, and AIRS are 4.2 %, 5.8 %, and 5.3 % in the altitude ranges of 20 to 27 km, respectively. However, the biases below 20 km are negative, which indicates the profile of CH4 from FTIR is less than the profiles derived from correlative instruments by −4.9 %, −1.8 %, and −2.8 %. The averaged positive bias between FTIR nitrous oxide and correlative instrument, MIPAS, in the altitude range of 20 to 27 km is 7.8 %, and a negative bias of −4 % at altitudes below 20 km. An averaged positive bias of 9.3 % in the altitude range of 17 to 27 km is obtained for FTIR N2O with MLS. In all the comparisons of CH4 from FTIR with data from MIPAS, MLS, and AIRS, sensors on board satellites indicate a negative bias below 20 km and a positive bias above 20 km. The mean error between partial-column amounts of methane from MIPAS and the ground-based FTIR is −5.5 %, with a standard deviation of 5 % that shows very good agreement as exhibited by relative differences between vertical profiles. Thus, the retrieved CH4 and N2O VMR and column amounts from Addis Ababa, tropical site, is found to exhibit very good agreement with all coincident satellite observations. Therefore, the bias obtained from the comparison is comparable to the precision of FTIR measurement, which allows the use of data in further scientific studies as it represents a unique environment of tropical Africa, a region poorly investigated in the past.

Description: In the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), the amplitudes and phases of the annual, semi-annual and quasi-biennial variation in stratospheric and lower mesospheric water were compared using 30 data sets from 13 different satellite instruments. These comparisons aimed to provide a comprehensive overview of the typical uncertainties in the observational database which can be considered in subsequent observational and modelling studies. For the amplitudes, a good agreement of their latitude and altitude distribution was found. Quantitatively there were differences in particular at high latitudes, close to the tropopause and in the lower mesosphere. In these regions, the standard deviation over all data sets typically exceeded 0.2 ppmv for the annual variation and 0.1 ppmv for the semi-annual and quasi-biennial variation. For the phase, larger differences between the data sets were found in the lower mesosphere. Generally the smallest phase uncertainties can be observed in regions where the amplitude of the variability is large. The standard deviations of the phases for all data sets were typically smaller than a month for the annual and semi-annual variation and smaller than 5 months for the quasi-biennial variation. The amplitude and phase differences among the data sets are caused by a combination of factors. In general, differences in the temporal variation of systematic errors and in the observational sampling play a dominant role. In addition, differences in the vertical resolution of the data, the considered time periods and influences of clouds, aerosols as well as non-local thermodynamic equilibrium (NLTE) effects cause differences between the individual data sets.

Description: 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.

Description: MIPAS thermal limb emission measurements were used to derive vertically resolved profiles of carbon tetrachloride (CCl4). Level-1b data versions MIPAS/5.02 to MIPAS/5.06 were converted into volume mixing ratio profiles using the level-2 processor developed at 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). Consideration of peroxyacetyl nitrate (PAN) as an interfering species, which is jointly retrieved, and CO2 line mixing is crucial for reliable retrievals. Parts of the CO2 Q-branch region that overlap with the CCl4 signature were omitted, since large residuals were still found even though line mixing was considered in the forward model. However, the omitted spectral region could be narrowed noticeably when line mixing was accounted for. A new CCl4 spectroscopic data set leads to slightly smaller CCl4 volume mixing ratios. In general, latitude–altitude cross sections show the expected CCl4 features with highest values of around 90 pptv at altitudes at and below the tropical tropopause and values decreasing with altitude and latitude due to stratospheric decomposition. Other patterns, such as subsidence in the polar vortex during winter and early spring, are also visible in the distributions. The decline in CCl4 abundance during the MIPAS Envisat measurement period (July 2002 to April 2012) is clearly reflected in the altitude–latitude cross section of trends estimated from the entire retrieved data set.

Description: In response to global warming, the Brewer–Dobson circulation in the stratosphere is expected to accelerate and the mean transport time of air along this circulation to decrease. This would imply a negative stratospheric age of air trend, i.e. an air parcel would need less time to travel from the tropopause to any point in the stratosphere. Age of air as inferred from tracer observations, however, shows zero to positive trends in the northern mid-latitude stratosphere and zonally asymmetric patterns. Using satellite observations and model calculations we show that the observed latitudinal and vertical patterns of the decadal changes of age of air in the lower to middle stratosphere during the period 2002–2012 are predominantly caused by a southward shift of the circulation pattern by about 5°. After correction for this shift, the observations reveal a hemispherically almost symmetric decrease of age of air in the lower to middle stratosphere up to 800 K of up to −0.25 years over the 2002–2012 period with strongest decrease in the northern tropics. This net change is consistent with long-term trends from model predictions.

Description: 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.

Description: In this paper we describe the stratospheric and mesospheric ozone (version V5r_O3_m22) distributions retrieved from MIPAS observations in the three middle atmosphere modes (MA, NLC, and UA) taken with an unapodized spectral resolution of 0.0625 cm−1 from 2005 until April 2012. O3 is retrieved from microwindows in the 14.8 and 10 µm spectral regions and requires non-local thermodynamic equilibrium (non-LTE) modelling of the O3 v1 and v3 vibrational levels. Ozone is reliably retrieved from 20 km in the MA mode (40 km for UA and NLC) up to ∼ 105 km during dark conditions and up to ∼ 95 km during illuminated conditions. Daytime MIPAS O3 has an average vertical resolution of 3–4 km below 70 km, 6–8 km at 70–80 km, 8–10 km at 80–90, and 5–7 km at the secondary maximum (90–100 km). For nighttime conditions, the vertical resolution is similar below 70 km and better in the upper mesosphere and lower thermosphere: 4–6 km at 70–100 km, 4–5 km at the secondary maximum, and 6–8 km at 100–105 km. The noise error for daytime conditions is typically smaller than 2 % below 50 km, 2–10 % between 50 and 70 km, 10–20 % at 70–90 km, and ∼ 30 % above 95 km. For nighttime, the noise errors are very similar below around 70 km but significantly smaller above, being 10–20 % at 75–95 km, 20–30 % at 95–100 km, and larger than 30 % above 100 km. The additional major O3 errors are the spectroscopic data uncertainties below 50 km (10–12 %) and the non-LTE and temperature errors above 70 km. The validation performed suggests that the spectroscopic errors below 50 km, mainly caused by the O3 air-broadened half-widths of the v2 band, are overestimated. The non-LTE error (including the uncertainty of atomic oxygen in nighttime) is relevant only above ∼ 85 km with values of 15–20 %. The temperature error varies from ∼ 3 % up to 80 km to 15–20 % near 100 km. Between 50 and 70 km, the pointing and spectroscopic errors are the dominant uncertainties. The validation performed in comparisons with SABER, GOMOS, MLS, SMILES, and ACE-FTS shows that MIPAS O3 has an accuracy better than 5 % at and below 50 km, with a positive bias of a few percent. In the 50–75 km region, MIPAS O3 has a positive bias of ≈ 10 %, which is possibly caused in part by O3 spectroscopic errors in the 10 µm region. Between 75 and 90 km, MIPAS nighttime O3 is in agreement with other instruments by 10 %, but for daytime the agreement is slightly larger, ∼ 10–20 %. Above 90 km, MIPAS daytime O3 is in agreement with other instruments by 10 %. At night, however, it shows a positive bias increasing from 10 % at 90 km to 20 % at 95–100 km, the latter of which is attributed to the large atomic oxygen abundance used. We also present MIPAS O3 distributions as function of altitude, latitude, and time, showing the major O3 features in the middle and upper mesosphere. In addition to the rapid diurnal variation due to photochemistry, the data also show apparent signatures of the diurnal migrating tide during both day- and nighttime, as well as the effects of the semi-annual oscillation above ∼ 70 km in the tropics and mid-latitudes. The tropical daytime O3 at 90 km shows a solar signature in phase with the solar cycle.