ALBERT

Description: Nitric acid (HNO3) is one of the key products that are operationally retrieved by the European Space Agency (ESA) from the emission spectra measured by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) onboard ENVISAT. The product version 4.61/4.62 for the observation period between July 2002 and March 2004 is validated by comparisons with a number of independent observations from ground-based stations, aircraft/balloon campaigns, and satellites. Individual HNO3 profiles of the ESA MIPAS level-2 product show good agreement with those of MIPAS-B and MIPAS-STR (the balloon and aircraft version of MIPAS, respectively), and the balloon-borne infrared spectrometers MkIV and SPIRALE, mostly matching the reference data within the combined instrument error bars. In most cases differences between the correlative measurement pairs are less than 1 ppbv (5–10%) throughout the entire altitude range up to about 38 km (~6 hPa), and below 0.5 ppbv (15–20% or more) above 30 km (~17 hPa). However, differences up to 4 ppbv compared to MkIV have been found at high latitudes in December 2002 in the presence of polar stratospheric clouds. The degree of consistency is further largely affected by the temporal and spatial coincidence, and differences of 2 ppbv may be observed between 22 and 26 km (~50 and 30 hPa) at high latitudes near the vortex boundary, due to large horizontal inhomogeneity of HNO3. Similar features are also observed in the mean differences of the MIPAS ESA HNO3 VMRs with respect to the ground-based FTIR measurements at five stations, aircraft-based SAFIRE-A and ASUR, and the balloon campaign IBEX. The mean relative differences between the MIPAS and FTIR HNO3 partial columns are within ±2%, comparable to the MIPAS systematic error of ~2%. %This should be the systematic error without spectroscopy since the ground-based data were retrieved using the same version of the HITRAN database. For the vertical profiles, the biases between the MIPAS and FTIR data are generally below 10% in the altitudes of 10 to 30 km. The MIPAS and SAFIRE chem{HNO_3} data generally match within their total error bars for the mid and high latitude flights, despite the larger atmospheric inhomogeneities that characterize the measurement scenario at higher latitudes. The MIPAS and ASUR comparison reveals generally good agreements better than 10–13% at 20–34 km. The MIPAS and IBEX measurements agree reasonably well (mean relative differences within ±15%) between 17 and 32 km. Statistical comparisons of the MIPAS profiles correlated with those of Odin/SMR, ILAS-II, and ACE-FTS generally show good consistency. The mean differences averaged over individual latitude bands or all bands are within the combined instrument errors, and generally within 1, 0.5, and 0.3 ppbv between 10 and 40 km (~260 and 4.5 hPa) for Odin/SMR, ILAS-II, and ACE-FTS, respectively. The standard deviations of the differences are between 1 to 2 ppbv. The standard deviations for the satellite comparisons and for almost all other comparisons are generally larger than the estimated measurement uncertainty. This is associated with the temporal and spatial coincidence error and the horizontal smoothing error which are not taken into account in our error budget. Both errors become large when the spatial variability of the target molecule is high.

Description: Simulations of CO, N2O and CH4 from a coupled chemistry-climate model (CMAM) are compared with satellite measurements from Odin Sub-Millimeter Radiometer (Odin/SMR), Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), and Aura Microwave Limb Sounder (Aura/MLS). Pressure-latitude cross-sections and seasonal time series demonstrate that CMAM reproduces the observed global distributions and the polar winter time evolutions of the CO, N2O, and CH4 measurements quite well. Generally, excellent agreement with measurements is found in CO monthly zonal mean profiles in the stratosphere and mesosphere for various latitudes and seasons. The difference between the simulations and the observations are generally within 30%, which is comparable with the difference between the instruments in the upper stratosphere and mesosphere. In general, the CO measurements also show an excellent agreement between themselves although MLS retrievals are noisier than other retrievals above 10 hPa (~32 km). The measurements also show large difference in the lower stratosphere and upper troposphere. Comparisons of N2O show that CMAM results usually have a less than 15% difference to the measurements in the lower and middle stratosphere, and the observations are consistent as well. However, the standard version of CMAM has a serious low bias in the upper stratosphere. The CMAM CH4 distribution is also close to the observations in the lower stratosphere, but has a similar but smaller negative bias in the upper stratosphere. These negative biases can be reduced by introducing a vertical diffusion coefficient related to gravity wave drag. CO measurements from 2004 and 2006 show evidence of enhanced descent of air from the mesosphere into the stratosphere in the Arctic after strong stratospheric sudden warmings (SSWs). CMAM also shows strong descent of air after SSWs, but further investigation is needed. In the tropics, CMAM captures the "tape recorder" (or annual oscillation) in the lower stratosphere and the semiannual oscillations (SAO) at the stratopause and mesopause shown in MLS CO and SMR N2O observations. The inter-annual variation of the SAO at the stratopause in SMR N2O observations also shows a biennial oscillation, but CMAM cannot does not reproduce this feature. However, this study confirms that CMAM is able to simulate middle atmospheric transport processes reasonably well.

Description: The wintertime abundance of nitric acid (HNO3) in the polar upper stratosphere displays a strong inter-annual variability, and is known to be strongly influenced by energetic particle precipitation, primarily during solar proton events, but also by precipitating electrons in the auroral zone. While wintertime HNO3 enhancements in the polar upper stratosphere had been occasionally observed before, from the ground or from satellite, we present here measurements by the Sub-Millimeter Radiometer instrument aboard the Odin satellite through 6 full annual cycles (2001 to 2007). Major solar proton events, e.g. during November 2001 or the Halloween solar storms of autumn 2003, lead to a two-stage HNO3 enhancement, likely involving different chemical reactions: a fast (about 1 week) in-situ enhancement from the mid to the upper stratosphere is followed by a slower, longer-lasting one, whereby anomalies originating in the upper stratosphere can descend within the polar vortex into the lower stratosphere. We highlight the fact that the actual chemical coupling between the upper and lower atmosphere involves a complex interplay of chemistry, dynamics and energetic particle precipitation.

Description: The Sub-Millimetre Radiometer (SMR) on board the Odin satellite, launched in February 2001, observes thermal emissions of stratospheric nitric acid (HNO3) originating from the Earth limb in a band centred at 544.6 GHz. Height-resolved measurements of the global distribution of nitric acid in the stratosphere between ~18–45 km (~1.5–60 hPa) were performed approximately on two observation days per week. An HNO3 climatology based on roughly 6 years of observations from August 2001 to December 2007 was created. The study highlights the spatial and seasonal variation of nitric acid in the stratosphere, characterised by a pronounced seasonal cycle at middle and high latitudes with maxima during late fall and minima during spring, strong denitrification in the lower stratosphere of the Antarctic polar vortex during winter (the irreversible removal of NOy by the sedimentation of cloud particles containing HNO3), as well as high quantities of HNO3 formed every winter at high-latitudes in the middle and upper stratosphere. A strong inter-annual variability is observed in particular at high latitudes. A comparison with a stratospheric HNO3 climatology based on UARS/MLS measurements from the 1990s shows a good consistency and agreement of the main morphological features in the potential temperature range ~465 to ~960 K, if the different characteristics of the data sets such as altitude range and resolution are considered.

Description: Mesospheric water vapour measurements taken by the SMR instrument onboard the Odin satellite between 2002 and 2006 have been analysed with focus on the mesospheric semi-annual circulation in the tropical and subtropical region. This analysis provides the first complete picture of mesospheric SAO in water vapour, covering altitudes above 80 km where the only previous study based on UARS/HALOE data was limited. Our analysis shows a clear semi-annual variation in the water vapour distribution in the entire altitude range between 65 km and 100 km in the equatorial area. Maxima occur near the equinoxes below 75 km and around the solstices above 80 km. The phase reversal occurs in the small layer in-between, consistent with the downward propagation of the mesospheric SAO in the zonal wind in this altitude range. The SAO amplitude exhibits a double peak structure, with maxima at about 75 km and 81 km. The observed amplitudes show higher values than the UARS/HALOE amplitudes. The upper peak amplitude remains relatively constant with latitude. The lower peak amplitude decreases towards higher latitudes, but recovers in the Southern Hemisphere subtropics. On the other hand, the annual variation is much more prominent in the northern hemispheric subtropics. Furthermore, higher volume mixing ratios during summer and lower values during winter are observed in the Northern Hemisphere subtropics, as compared to the corresponding latitude range in the Southern Hemisphere.

Description: Five years of OSIRIS (Optical Spectrograph and InfraRed Imager System) NO2 and SMR (Sub-Millimetre Radiometer) HNO3 observations from the Odin satellite, combined with data from a photochemical box model, have been used to construct a stratospheric proxy NOy data set including the gases: NO, NO2, HNO3, 2×N2O5 and CIONO2. This Odin NOy climatology is based on all daytime measurements and contains monthly mean and standard deviation, expressed as mixing ratio or number density, as function of latitude or equivalent latitude (5° bins) on 17 vertical layers (altitude, pressure or potential temperature) between 14 and 46 km. Comparisons with coincident NOy profiles from the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE-FTS) instrument were used to evaluate several methods to combine Odin observations with model data. This comparison indicates that the most appropriate merging technique uses OSIRIS measurements of NO2, scaled with model NO/NO2 ratios, to estimate NO. The sum of 2×N2O5 and CIONO2 is estimated from uncertainty-based weighted averages of scaled observations of SMR HNO3 and OSIRIS NO2. Comparisons with ACE-FTS suggest the precision (random error) and accuracy (systematic error) of Odin NOy profiles are about 15% and 20%, respectively. Further comparisons between Odin and the Canadian Middle Atmosphere Model (CMAM) show agreement to within 20% and 2 ppb throughout most of the stratosphere except in the polar vortices. A particularly large disagreement within the Antarctic vortex in the upper stratosphere during spring indicates too strong descent of air in CMAM. The combination of good temporal and spatial coverage, a relatively long data record, and good accuracy and precision make this a valuable NOy product for various atmospheric studies and model assessments.

Description: The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Water vapour (H2O), one of the most important molecules for climate and atmospheric chemistry, is one of the key species provided by the two principal instruments, the infrared Fourier Transform Spectrometer (ACE-FTS) and the MAESTRO UV-Visible spectrometer (ACE-MAESTRO). The first instrument performs measurements on several lines in the 1362–2137 cm−1 range, from which vertically resolved H2O concentration profiles are retrieved, from 7 to 90 km altitude. ACE-MAESTRO measures profiles using the water absorption band in the near infrared part of the spectrum at 926.0–969.7 nm. This paper presents a comprehensive validation of the ACE-FTS profiles. We have compared the H2O volume mixing ratio profiles with space-borne (SAGE II, HALOE, POAM III, MIPAS, SMR) observations and measurements from balloon-borne frostpoint hygrometers and a ground based lidar. We show that the ACE-FTS measurements provide H2O profiles with small retrieval uncertainties in the stratosphere (better than 5% from 15 to 70 km, gradually increasing above). The situation is unclear in the upper troposphere, due mainly to the high variability of the water vapour volume mixing ratio in this region. A new water vapour data product from the ACE-MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) is also presented and initial comparisons with ACE-FTS are discussed.

Description: The Atmospheric Chemistry Experiment (ACE), also known as SCISAT, was launched on 12 August 2003, carrying two instruments that measure vertical profiles of atmospheric constituents using the solar occultation technique. One of these instruments, the ACE Fourier Transform Spectrometer (ACE-FTS), is measuring volume mixing ratio (VMR) profiles of nitrous oxide (N2O) from the upper troposphere to the lower mesosphere at a vertical resolution of about 3–4 km. In this study, the quality of the ACE-FTS version 2.2 N2O data is assessed through comparisons with coincident measurements made by other satellite, balloon-borne, aircraft, and ground-based instruments. These consist of vertical profile comparisons with the SMR, MLS, and MIPAS satellite instruments, multiple aircraft flights of ASUR, and single balloon flights of SPIRALE and FIRS-2, and partial column comparisons with a network of ground-based Fourier Transform InfraRed spectrometers (FTIRs). Overall, the quality of the ACE-FTS version 2.2 N2O VMR profiles is good over the entire altitude range from 5 to 60 km. Between 6 and 30 km, the mean absolute differences for the satellite comparisons lie between −42 ppbv and +17 ppbv, with most within ±20 ppbv. This corresponds to relative deviations from the mean that are within ±15%, except for comparisons with MIPAS near 30 km, for which they are as large as 22.5%. Between 18 and 30 km, the mean absolute differences are generally within ±10 ppbv, again excluding the aircraft and balloon comparisons. From 30 to 60 km, the mean absolute differences are within ±4 ppbv, and are mostly between −2 and +1 ppbv. Given the small N2O VMR in this region, the relative deviations from the mean are therefore large at these altitudes, with most suggesting a negative bias in the ACE-FTS data between 30 and 50 km. In the comparisons with the FTIRs, the mean relative differences between the ACE-FTS and FTIR partial columns are within ±6.6% for eleven of the twelve contributing stations. This mean relative difference is negative at ten stations, suggesting a small negative bias in the ACE-FTS partial columns over the altitude regions compared. Excellent correlation (R=0.964) is observed between the ACE-FTS and FTIR partial columns, with a slope of 1.01 and an intercept of −0.20 on the line fitted to the data.

Description: The Atmospheric Chemistry Experiment (ACE) satellite was launched on 12 August 2003. Its two instruments measure vertical profiles of over 30 atmospheric trace gases by analyzing solar occultation spectra in the ultraviolet/visible and infrared wavelength regions. The reservoir gases HNO3, ClONO2, and N2O5 are three of the key species provided by the primary instrument, the ACE Fourier Transform Spectrometer (ACE-FTS). This paper describes the ACE-FTS version 2.2 data products, including the N2O5 update, for the three species and presents validation comparisons with available observations. We have compared volume mixing ratio (VMR) profiles of HNO3, ClONO2, and N2O5 with measurements by other satellite instruments (SMR, MLS, MIPAS), aircraft measurements (ASUR), and single balloon-flights (SPIRALE, FIRS-2). Partial columns of HNO3 and ClONO2 were also compared with measurements by ground-based Fourier Transform Infrared (FTIR) spectrometers. Overall the quality of the ACE-FTS v2.2 HNO3 VMR profiles is good from 18 to 35 km. For the statistical satellite comparisons, the mean absolute differences are generally within ±1 ppbv (±20%) from 18 to 35 km. For MIPAS and MLS comparisons only, mean relative differences lie within ±10% between 10 and 36 km. ACE-FTS HNO3 partial columns (~15–30 km) show a slight negative bias of −1.3% relative to the ground-based FTIRs at latitudes ranging from 77.8° S–76.5° N. Good agreement between ACE-FTS ClONO2 and MIPAS, using the Institut für Meteorologie und Klimaforschung and Instituto de Astrofísica de Andalucía (IMK-IAA) data processor is seen. Mean absolute differences are typically within ±0.01 ppbv between 16 and 27 km and less than +0.09 ppbv between 27 and 34 km. The ClONO2 partial column comparisons show varying degrees of agreement, depending on the location and the quality of the FTIR measurements. Good agreement was found for the comparisons with the midlatitude Jungfraujoch partial columns for which the mean relative difference is 4.7%. ACE-FTS N2O5 has a low bias relative to MIPAS IMK-IAA, reaching −0.25 ppbv at the altitude of the N2O5 maximum (around 30 km). Mean absolute differences at lower altitudes (16–27 km) are typically −0.05 ppbv for MIPAS nighttime and ±0.02 ppbv for MIPAS daytime measurements.

Description: This paper presents extensive validation analyses of ozone observations from the Atmospheric Chemistry Experiment (ACE) satellite instruments: the ACE Fourier Transform Spectrometer (ACE-FTS) and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) instrument. The ACE satellite instruments operate in the mid-infrared and ultraviolet-visible-near-infrared spectral regions using the solar occultation technique. In order to continue the long-standing record of solar occultation measurements from space, a detailed quality assessment is required to evaluate the ACE data and validate their use for scientific purposes. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from satellite-borne, airborne, balloon-borne and ground-based instruments, by analysing volume mixing ratio profiles and partial column densities. The ACE-FTS version 2.2 Ozone Update product reports more ozone than most correlative measurements from the upper troposphere to the lower mesosphere. At altitude levels from 16 to 44 km, the mean differences range generally between 0 and +10% with a slight but systematic positive bias (typically +5%). At higher altitudes (45–60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments by up to ~40% (typically +20%). For the ACE-MAESTRO version 1.2 ozone data product, agreement within ±10% (generally better than ±5%) is found between 18 and 40 km for the sunrise and sunset measurements. At higher altitudes (45–55 km), systematic biases of opposite sign are found between the ACE-MAESTRO sunrise and sunset observations. While ozone amounts derived from the ACE-MAESTRO sunrise occultation data are often smaller than the coincident observations (by as much as −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS and indicate a large positive bias (+10 to +30%) in this altitude range. In contrast, there is no significant difference in bias found for the ACE-FTS sunrise and sunset measurements. These systematic effects in the ozone profiles retrieved from the measurements of ACE-FTS and ACE-MAESTRO are being investigated. This work shows that the ACE instruments provide reliable, high quality measurements from the tropopause to the upper stratosphere and can be used with confidence in this vertical domain.