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A new algorithm to derive near-real-time (NRT) data products for the Aura Microwave Limb Sounder (MLS) is presented. The old approach was based on a simplified optimal estimation retrieval algorithm (OE-NRT) to reduce computational demands and latency. This paper describes the setup, training, and evaluation of a redesigned approach based on artificial neural networks (ANN-NRT), which is trained on >17 years of MLS radiance observations and composition profile retrievals. Comparisons of joint histograms and performance metrics derived between the two NRT results and the operational MLS products demonstrate a noticeable statistical improvement from ANN-NRT. This new approach results in higher correlation coefficients, in addition to lower root-mean-square deviations and biases at almost all retrieval levels compared to OE-NRT. The exceptions are pressure levels with concentrations close to 0 ppbv (parts per billion by volume), where the ANN models fail to establish a functional relationship and tend to predict 0. Depending on the application, this behavior might be advantageous. While the developed models can take advantage of the extended MLS data record, this study demonstrates that training ANN-NRT on just a single year of MLS observations is sufficient to improve upon OE-NRT. This confirms the potential of applying machine learning to the NRT efforts of other current and future mission concepts.

Using Aura Microwave Limb Sounder satellite observations of stratospheric nitrous oxide (N2O), ozone, and temperature from 2005 through 2021, we calculate the atmospheric lifetime of N2O to be decreasing at a rate of −2.1 ± 1.2 %/decade. This decrease is occurring because the N2O abundances in the middle tropical stratosphere, where N2O is photochemically destroyed, are increasing at a faster rate than the bulk N2O in the lower atmosphere. The cause appears to be a more vigorous stratospheric circulation, which models predict to be a result of climate change. If the observed trends in lifetime and implied emissions continue, then the change in N2O over the 21st century will be 27 % less than those projected with a fixed lifetime, and the impact on global warming and ozone depletion will be proportionately lessened. Because global warming is caused in part by N2O, this finding is an example of a negative climate–chemistry feedback.

We analyze Aura Microwave Limb Sounder (MLS) monthly zonal mean time series of ClO and HOCl between 50∘ S and 50∘ N to estimate upper stratospheric trends in these chlorine species from 2005 through 2020. We compare these observations to those from the Whole Atmosphere Community Climate Model version 6 (WACCM6), run under the specified dynamics configuration. The model sampling follows the MLS coverage in space and local time. We use version 5 MLS ClO zonal mean daytime profiles and similarly binned daytime ClO model profiles from 32 to 1.5 hPa. For MLS HOCl, we use the version 5 offline product derived from daily zonal mean radiances rather than averaged level-2 profiles; MLS HOCl is scientifically useful between 10 and 2 hPa, and the HOCl monthly zonal means are separated into day and night for comparison to WACCM6. We find good agreement (mostly within ∼ 10 %) between the climatological MLS ClO daytime distributions and the model ClO climatology for 2005–2020. The model HOCl climatology, however, underestimates the MLS HOCl climatology by about 30 %. This could well be caused by a combination of fairly large systematic uncertainties in both the model-assumed rate constant for the formation of HOCl and the MLS HOCl retrievals themselves. The model daytime ClO trends versus latitude and pressure agree quite well with those from MLS. MLS-derived near-global upper stratospheric daytime trends between 7 and 2 hPa are −0.73 ± 0.40 % yr−1 for ClO and −0.39 ± 0.35 % yr−1 for HOCl, with 2σ uncertainty estimates used here. The corresponding model decreases are somewhat faster than observed (although the difference is not statistically significant), with trend values of −0.85 ± 0.45 % yr−1 for ClO and −0.64 ± 0.37 % yr−1 for HOCl. Both data and model results point to a faster trend in ClO than in HOCl. The MLS ClO trends are consistent with past estimates of upper stratospheric ClO trends from satellite and ground-based microwave data. As discussed in the past, trends in other species (in particular, positive trends in CH4 and H2O) can lead to a ClO decrease that is faster than the decrease in total inorganic chlorine. Regarding trends in HOCl, positive trends in HO2 can lead to a faster rate of formation for HOCl as a function of time, which partially offsets the decreasing trend in active chlorine. The decreasing trends in upper stratospheric ClO and HOCl provide additional confirmation of the effectiveness of the Montreal Protocol and its amendments, which have led to the early stages of an expected long-term ozone recovery from the effects of ozone-depleting substances.

An improved cloud detection algorithm for the Aura Microwave Limb Sounder (MLS) is presented. This new algorithm is based on a feedforward artificial neural network and uses as input, for each MLS limb scan, a vector consisting of 1710 brightness temperatures provided by MLS observations from 15 different tangent altitudes and up to 13 spectral channels in each of 10 different MLS bands. The model has been trained on global cloud properties reported by Aqua's Moderate Resolution Imaging Spectroradiometer (MODIS). In total, the colocated MLS–MODIS data set consists of 162 117 combined scenes sampled on 208 d over 2005–2020. A comparison to the current MLS cloudiness flag used in “Level 2” processing reveals a huge improvement in classification performance. For previously unseen data, the algorithm successfully detects > 93 % of profiles affected by clouds, up from ∼ 16 % for the Level 2 flagging. At the same time, false positives reported for actually clear profiles are comparable to the Level 2 results. The classification performance is not dependent on geolocation but slightly decreases over low-cloud-cover regions. The new cloudiness flag is applied to determine average global cloud cover maps over 2015–2019, successfully reproducing the spatial patterns of mid-level to high clouds seen in MODIS data. It is also applied to four example cloud fields to illustrate its reliable performance for different cloud structures with varying degrees of complexity. Training a similar model on MODIS-retrieved cloud top pressure (pCT) yields reliable predictions with correlation coefficients > 0.82. It is shown that the model can correctly identify > 85 % of profiles with pCT < 400 hPa. Similar to the cloud classification model, global maps and example cloud fields are provided, which reveal good agreement with MODIS results. The combination of the cloudiness flag and predicted cloud top pressure provides the means to identify MLS profiles in the presence of high-reaching convection.

Forest fires in British Columbia in August 2017 caused a pyrocumulonimbus event that injected a polluted air mass into the lower stratosphere. The Microwave Limb Sounder (MLS) on the Aura satellite first observed the polluted air mass on 14 August 2017 and continued to observe it for 60 d (100 d in water vapour). We estimate the mass of CO injected into the stratosphere to be 2400 Gg. Events in which a fire injects its burning products directly into the stratosphere are rare: this is the third of four such events in the 16 years since the launch of Aura, the second largest of the four events, and the only one in the Northern Hemisphere. The other three events occurred in Australia in December 2006, February 2009 and from December 2019 to January 2020. Unlike the 2006 and 2009 events, but like the 2019–2020 event, the polluted air mass described here had a clearly elevated water vapour content: between 2.5 and 5 times greater than that in the surrounding atmosphere. We describe the evolution of the polluted air mass, showing that it rose to an altitude of about 24 km (31 hPa) and divided into several identifiable parts. In addition to CO and H2O, we observe enhanced amounts of HCN, CH3CN, CH3Cl and CH3OH with mixing ratios in the range to be expected from a variety of measurements in other biomass burning plumes. We use back trajectories and plume-dispersion modelling to demonstrate that the pollutants observed by MLS originated in the British Columbia fires, the likeliest source being at 53.2∘ N, 121.8∘ W at 05:20 UTC on 13 August 2017.

The Microwave Limb Sounder (MLS), launched on NASA's Aura spacecraft in 2004, measures vertical profiles of the abundances of key atmospheric species from the upper troposphere to the mesosphere with daily near-global coverage. We review the first 15 years of the record of H2O and N2O measurements from the MLS 190 GHz subsystem (along with other 190 GHz information), with a focus on their long-term stability, largely based on comparisons with measurements from other sensors. These comparisons generally show signs of an increasing drift in the MLS “version 4” (v4) H2O record starting around 2010. Specifically, comparisons with v4.1 measurements from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) indicate a ∼ 2 %–3 % per decade drift over much of the stratosphere, increasing to as much as ∼ 7 % per decade around 46 hPa. Larger drifts, of around 7 %–11 % per decade, are seen in comparisons to balloon-borne frost point hygrometer measurements in the lower stratosphere. Microphysical calculations considering the formation of polar stratospheric clouds in the Antarctic winter stratosphere corroborate a drift in MLS v4 water vapor measurements in that region and season. In contrast, comparisons with the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument on NASA's Thermosphere Ionosphere Mesosphere Energetics and Dynamics (TIMED) mission, and with ground-based Water Vapor Millimeter-wave Spectrometer (WVMS) instruments, do not show statistically significant drifts. However, the uncertainty in these comparisons is large enough to encompass most of the drifts identified in other comparisons. In parallel, the MLS v4 N2O product is shown to be generally decreasing over the same period (when an increase in stratospheric N2O is expected, reflecting a secular growth in emissions), with a more pronounced drift in the lower stratosphere than that found for H2O. Comparisons to ACE-FTS and to MLS N2O observations in a different spectral region, with the latter available from 2004 to 2013, indicate an altitude-dependent drift, growing from 5 % per decade or less in the mid-stratosphere to as much as 15 % per decade in the lower stratosphere. Detailed investigations of the behavior of the MLS 190 GHz subsystem reveal a drift in its “sideband fraction” (the relative sensitivity of the 190 GHz receiver to the two different parts of the microwave spectrum that it observes). Our studies indicate that sideband fraction drift accounts for much of the observed changes in the MLS H2O product and some portion of the changes seen in N2O. The 190 GHz sideband fraction drift has been corrected in the new “version 5” (v5) MLS algorithms, which have now been used to reprocess the entire MLS record. As a result of this correction, the MLS v5 H2O record shows no statistically significant drifts compared to ACE-FTS. However, statistically significant drifts remain between MLS v5 and frost point measurements, although they are reduced. Drifts in v5 N2O are about half the size of those in v4 but remain statistically significant. Scientists are advised to use MLS v5 data in all future studies. Quantification of interregional and seasonal to annual changes in MLS H2O and N2O will not be affected by the drift. However, caution is advised in studies using the MLS record to examine long-term (multiyear) variability and trends in either of these species, especially N2O; such studies should only be undertaken in consultation with the MLS team. Importantly, this drift does not affect any of the MLS observations made in other spectral regions such as O3, HCl, CO, ClO, or temperature.

Hydrogen chloride (HCl) is the most abundant (more than 95 %) among inorganic chlorine compounds Cly in the upper stratosphere. The HCl molecule is observed to obtain long-term quantitative estimations of the total budget of the stratospheric chlorine compounds. In this study, we provided HCl vertical profiles at altitudes of 16–100 km using the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) from space. The HCl vertical profile from the upper troposphere to the lower thermosphere is reported for the first time from SMILES observations; the data quality is quantified by comparison with other measurements and via theoretical error analysis. We used the SMILES level-2 research product version 3.0.0. The period of the SMILES HCl observation was from 12 October 2009 to 21 April 2010, and the latitude coverage was 40∘ S–65∘ N. The average HCl vertical profile showed an increase with altitude up to the stratopause (∼ 45 km), approximately constant values between the stratopause and the upper mesosphere (∼ 80 km), and a decrease from the mesopause to the lower thermosphere (∼ 100 km). This behavior was observed in all latitude regions and reproduced by the Whole Atmosphere Community Climate Model in the specified dynamics configuration (SD-WACCM). We compared the SMILES HCl vertical profiles in the stratosphere and lower mesosphere with HCl profiles from Microwave Limb Sounder (MLS) on the Aura satellite, as well as from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT and the TErahertz and submillimeter LImb Sounder (TELIS) (balloon borne). The TELIS observations were performed using the superconductive limb emission technique, as used by SMILES. The globally averaged vertical HCl profiles of SMILES agreed well with those of MLS and ACE-FTS within 0.25 and 0.2 ppbv between 20 and 40 km (within 10 % between 30 and 40 km; there is a larger discrepancy below 30 km), respectively. The SMILES HCl concentration was smaller than those of MLS and ACE-FTS as the altitude increased from 40 km, and the difference was approximately 0.4–0.5 ppbv (12 %–15 %) at 50–60 km. The difference between SMILES and TELIS HCl observations was about 0.3 ppbv in the polar winter region between 20 and 34 km, except near 26 km. SMILES HCl error sources that may cause discrepancies with the other observations are investigated by a theoretical error analysis. We calculated errors caused by the uncertainties of spectroscopic parameters, instrument functions, and atmospheric temperature profiles. The Jacobian for the temperature explains the negative bias of the SMILES HCl concentrations at 50–60 km.

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.

The Tropospheric Emission Spectrometer (TES) on the A-Train Aura satellite was designed to profile tropospheric ozone and its precursors, taking measurements from 2004 to 2018. Starting in 2008, TES global sampling of tropospheric ozone was gradually reduced in latitude, with global coverage stopping in 2011. To extend the record of TES, this work presents a multispectral approach that will provide O3 data products with vertical resolution and measurement error similar to TES by combining the single-footprint thermal infrared (TIR) hyperspectral radiances from the Aqua Atmospheric Infrared Sounder (AIRS) instrument and the ultraviolet (UV) channels from the Aura Ozone Monitoring Instrument (OMI). The joint AIRS+OMI O3 retrievals are processed through the MUlti-SpEctra, MUlti-SpEcies, MUlti-SEnsors (MUSES) retrieval algorithm. Comparisons of collocated joint AIRS+OMI and TES to ozonesonde measurements show that both systems have similar errors, with mean and standard deviation of the differences well within the estimated measurement error. AIRS+OMI and TES have slightly different biases (within 5 parts per billion) vs. the sondes. Both AIRS and OMI have wide swath widths ( ∼ 1650 km for AIRS; ∼ 2600 km for OMI) across satellite ground tracks. Consequently, the joint AIRS+OMI measurements have the potential to maintain TES vertical sensitivity while increasing coverage by 2 orders of magnitude, thus providing an unprecedented new data set with which to quantify the evolution of tropospheric ozone.

This study investigates orbital sampling biases and evaluates the additional impact caused by data quality screening for the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and the Aura Microwave Limb Sounder (MLS). MIPAS acts as a proxy for typical infrared limb emission sounders, while MLS acts as a proxy for microwave limb sounders. These biases were calculated for temperature and several trace gases by interpolating model fields to real sampling patterns and, additionally, screening those locations as directed by their corresponding quality criteria. Both instruments have dense uniform sampling patterns typical of limb emission sounders, producing almost identical sampling biases. However, there is a substantial difference between the number of locations discarded. MIPAS, as a mid-infrared instrument, is very sensitive to clouds, and measurements affected by them are thus rejected from the analysis. For example, in the tropics, the MIPAS yield is strongly affected by clouds, while MLS is mostly unaffected. The results show that upper-tropospheric sampling biases in zonally averaged data, for both instruments, can be up to 10 to 30 %, depending on the species, and up to 3 K for temperature. For MIPAS, the sampling reduction due to quality screening worsens the biases, leading to values as large as 30 to 100 % for the trace gases and expanding the 3 K bias region for temperature. This type of sampling bias is largely induced by the geophysical origins of the screening (e.g. clouds). Further, analysis of long-term time series reveals that these additional quality screening biases may affect the ability to accurately detect upper-tropospheric long-term changes using such data. In contrast, MLS data quality screening removes sufficiently few points that no additional bias is introduced, although its penetration is limited to the upper troposphere, while MIPAS may cover well into the mid-troposphere in cloud-free scenarios. We emphasize that the results of this study refer only to the representativeness of the respective data, not to their intrinsic quality.

It is known from ground-based measurements made during the 1982–1983 and 1997–1998 El Niño events that atmospheric hydrogen cyanide (HCN) tends to be higher during such years than at other times. The Microwave Limb Sounder (MLS) on the Aura satellite has been measuring HCN mixing ratios since launch in 2004; the measurements are ongoing at the time of writing. The winter of 2015–2016 saw the largest El Niño event since 1997–1998. We present MLS measurements of HCN in the lower stratosphere for the Aura mission to date, comparing the 2015–2016 El Niño period to the rest of the mission. HCN in 2015–2016 is higher than at any other time during the mission, but ground-based measurements suggest that it may have been even more elevated in 1997–1998. As the MLS HCN data are essentially unvalidated, we show them alongside data from the MIPAS and ACE-FTS instruments; the three instruments agree reasonably well in the tropical lower stratosphere. Global HCN emissions calculated from the Global Fire Emissions Database (GFED v4.1) database are much greater during large El Niño events and are greater in 1997–1998 than in 2015–2016, thereby showing good qualitative agreement with the measurements. Correlation between El Niño–Southern Oscillation (ENSO) indices, measured HCN, and GFED HCN emissions is less clear if the 2015–2016 event is excluded. In particular, the 2009–2010 winter had fairly strong El Niño conditions and fairly large GFED HCN emissions, but very little effect is observed in the MLS HCN.

We use satellite-borne measurements collected over the last decade (2006–2015) from the Aura Microwave Limb Sounder (MLS) and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) to investigate the nitric acid distribution and the properties of polar stratospheric clouds (PSCs) in the early winter Antarctic vortex. Frequently, at the very start of the winter, we find that synoptic-scale depletion of HNO3 can be detected in the inner vortex before the first lidar detection of geophysically associated PSCs. The generation of "sub-visible" PSCs can be explained as arising from the development of a solid particle population with low number densities and large particle sizes. Assumed to be composed of nitric acid trihydrate (NAT), the sub-visible PSCs form at ambient temperatures well above the ice frost point, but also above the temperature at which supercooled ternary solution (STS) grows out of the background supercooled binary solution (SBS) distribution. The temperature regime of their formation, inferred from the simultaneous uptake of ambient HNO3 into NAT and their Lagrangian temperature histories, is at a depression of a few kelvin with respect to the NAT existence threshold, TNAT. Therefore, their nucleation requires a considerable supersaturation of HNO3 over NAT, and is consistent with a recently described heterogeneous nucleation process on solid foreign nuclei immersed in liquid aerosol. We make a detailed investigation of the comparative limits of detection of PSCs and the resulting sequestration of HNO3 imposed by lidar, mid-infrared, and microwave techniques. We find that the temperature history of air parcels, in addition to the local ambient temperature, is an important factor in the relative frequency of formation of liquid/solid PSCs. We conclude that the initiation of NAT nucleation and the subsequent development of large NAT particles capable of sedimentation and denitrification in the early winter do not emanate from an ice-seeding process. Finally, we investigate the patterns of interannual variability and compare the relative formation frequency of liquid and solid PSCs in the Antarctic lower polar stratosphere using the results of a cluster analysis to synthesize the combined CALIOP and MLS measurements into a relatively small number of interrelated categories.

This study investigates the representativeness of two types of orbital sampling applied to stratospheric temperature and trace gas fields. Model fields are sampled using real sampling patterns from the Aura Microwave Limb Sounder (MLS), the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). The MLS sampling acts as a proxy for a dense uniform sampling pattern typical of limb emission sounders, while HALOE and ACE-FTS represent coarse nonuniform sampling patterns characteristic of solar occultation instruments. First, this study revisits the impact of sampling patterns in terms of the sampling bias, as previous studies have done. Then, it quantifies the impact of different sampling patterns on the estimation of trends and their associated detectability. In general, we find that coarse nonuniform sampling patterns may introduce non-negligible errors in the inferred magnitude of temperature and trace gas trends and necessitate considerably longer records for their definitive detection. Lastly, we explore the impact of these sampling patterns on tropical vertical velocities derived from stratospheric water vapor measurements. We find that coarse nonuniform sampling may lead to a biased depiction of the tropical vertical velocities and, hence, to a biased estimation of the impact of the mechanisms that modulate these velocities. These case studies suggest that dense uniform sampling such as that available from limb emission sounders provides much greater fidelity in detecting signals of stratospheric change (for example, fingerprints of greenhouse gas warming and stratospheric ozone recovery) than coarse nonuniform sampling such as that of solar occultation instruments.

We validate Aura Microwave Limb Sounder (MLS) version 3 (v3) and version 4 (v4) retrievals of summertime temperature, water vapour and ozone in the upper troposphere and lower–middle stratosphere (UTLS; 10–316 hPa) against balloon soundings collected during the Study of Ozone, Aerosols and Radiation over the Tibetan Plateau (SOAR-TP). Mean v3 and v4 profiles of temperature, water vapour and ozone in this region during the measurement campaigns are almost identical through most of the stratosphere (10–68 hPa), but differ in several respects in the upper troposphere and tropopause layer. Differences in v4 relative to v3 include slightly colder mean temperatures from 100 to 316 hPa, smaller mean water vapour mixing ratios in the upper troposphere (215–316 hPa) and a more vertically homogeneous profile of mean ozone mixing ratios below the climatological tropopause (100–316 hPa). These changes substantially improve agreement between ozonesondes and MLS ozone retrievals in the upper troposphere, but slightly worsen existing cold and dry biases at these levels. Aura MLS temperature profiles contain significant cold biases relative to collocated temperature measurements in several layers of the lower–middle stratosphere and in the upper troposphere. MLS retrievals of water vapour volume mixing ratio generally compare well with collocated measurements, excepting a substantial dry bias (−32 ± 11 % in v4) that extends through most of the upper troposphere (121–261 hPa). MLS retrievals of ozone volume mixing ratio are biased high relative to collocated ozonesondes in the stratosphere (18–83 hPa), but are biased low at 100 hPa. The largest relative biases in ozone retrievals (approximately +70 %) are located at 83 hPa. MLS v4 offers substantial benefits relative to v3, particularly with respect to water vapour and ozone. Key improvements include larger data yields, reduced noise in the upper troposphere and smaller fluctuations in the bias profile at pressures larger than 100 hPa. The situation for temperature is less clear, with cold biases and noise levels in the upper troposphere, both larger in v4 than in v3. Several aspects of our results differ from those of validations conducted in other locations. These differences are often amplified by monsoon onset, indicating that the Asian monsoon anticyclone poses unique challenges for remote sensing that impact the quality of MLS retrievals in this region.

This study evaluates the distribution and variation of carbon monoxide (CO) in the upper troposphere and lower stratosphere (UTLS) during 2004–2012 as simulated by two chemical transport models, using the latest version of Aura Microwave Limb Sounder (MLS) observations. The simulated spatial distributions, temporal variations and vertical transport of CO in the UTLS region are compared with those observed by MLS. We also investigate the impact of surface emissions and deep convection on CO concentrations in the UTLS over different regions, using both model simulations and MLS observations. Global Modeling Initiative (GMI) and GEOS-Chem simulations of UTLS CO both show similar spatial distributions to observations. The global mean CO values simulated by both models agree with MLS observations at 215 and 147 hPa, but are significantly underestimated by more than 40 % at 100 hPa. In addition, the models underestimate the peak CO values by up to 70 % at 100 hPa, 60 % at 147 hPa and 40 % at 215 hPa, with GEOS-Chem generally simulating more CO at 100 hPa and less CO at 215 hPa than GMI. The seasonal distributions of CO simulated by both models are in better agreement with MLS in the Southern Hemisphere (SH) than in the Northern Hemisphere (NH), with disagreements between model and observations over enhanced CO regions such as southern Africa. The simulated vertical transport of CO shows better agreement with MLS in the tropics and the SH subtropics than the NH subtropics. We also examine regional variations in the relationships among surface CO emission, convection and UTLS CO concentrations. The two models exhibit emission–convection–CO relationships similar to those observed by MLS over the tropics and some regions with enhanced UTLS CO.

The well-established "Match" approach to quantifying chemical destruction of ozone in the polar lower stratosphere is applied to ozone observations from the Microwave Limb Sounder (MLS) on NASA's Aura spacecraft. Quantification of ozone loss requires distinguishing transport- and chemically induced changes in ozone abundance. This is accomplished in the Match approach by examining cases where trajectories indicate that the same air mass has been observed on multiple occasions. The method was pioneered using ozonesonde observations, for which hundreds of matched ozone observations per winter are typically available. The dense coverage of the MLS measurements, particularly at polar latitudes, allows matches to be made to thousands of observations each day. This study is enabled by recently developed MLS Lagrangian trajectory diagnostic (LTD) support products. Sensitivity studies indicate that the largest influence on the ozone loss estimates are the value of potential vorticity (PV) used to define the edge of the polar vortex (within which matched observations must lie) and the degree to which the PV of an air mass is allowed to vary between matched observations. Applying Match calculations to MLS observations of nitrous oxide, a long-lived tracer whose expected rate of change is negligible on the weekly to monthly timescales considered here, enables quantification of the impact of transport errors on the Match-based ozone loss estimates. Our loss estimates are generally in agreement with previous estimates for selected Arctic winters, though indicating smaller losses than many other studies. Arctic ozone losses are greatest during the 2010/11 winter, as seen in prior studies, with 2.0 ppmv (parts per million by volume) loss estimated at 450 K potential temperature (~ 18 km altitude). As expected, Antarctic winter ozone losses are consistently greater than those for the Arctic, with less interannual variability (e.g., ranging between 2.3 and 3.0 ppmv at 450 K). This study exemplifies the insights into atmospheric processes that can be obtained by applying the Match methodology to a densely sampled observation record such as that from Aura MLS.

We describe the publicly available data from the Global OZone Chemistry And Related trace gas Data records for the Stratosphere (GOZCARDS) project and provide some results, with a focus on hydrogen chloride (HCl), water vapor (H2O), and ozone (O3). This data set is a global long-term stratospheric Earth system data record, consisting of monthly zonal mean time series starting as early as 1979. The data records are based on high-quality measurements from several NASA satellite instruments and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) on SCISAT. We examine consistency aspects between the various data sets. To merge ozone records, the time series are debiased relative to SAGE II (Stratospheric Aerosol and Gas Experiments) values by calculating average offsets versus SAGE II during measurement overlap periods, whereas for other species the merging derives from an averaging procedure during overlap periods. The GOZCARDS files contain mixing ratios on a common pressure–latitude grid, as well as standard errors and other diagnostics; we also present estimates of systematic uncertainties in the merged products. Monthly mean temperatures for GOZCARDS were also produced, based directly on data from the Modern-Era Retrospective analysis for Research and Applications. The GOZCARDS HCl merged product comes from the Halogen Occultation Experiment (HALOE), ACE-FTS and lower-stratospheric Aura Microwave Limb Sounder (MLS) data. After a rapid rise in upper-stratospheric HCl in the early 1990s, the rate of decrease in this region for 1997–2010 was between 0.4 and 0.7 % yr−1. On 6–8-year timescales, the rate of decrease peaked in 2004–2005 at about 1 % yr−1, and it has since levelled off, at ~ 0.5 % yr−1. With a delay of 6–7 years, these changes roughly follow total surface chlorine, whose behavior versus time arises from inhomogeneous changes in the source gases. Since the late 1990s, HCl decreases in the lower stratosphere have occurred with pronounced latitudinal variability at rates sometimes exceeding 1–2 % yr−1. Recent short-term tendencies of lower-stratospheric and column HCl vary substantially, with increases from 2005 to 2010 for northern midlatitudes and deep tropics, but decreases (increases) after 2011 at northern (southern) midlatitudes. For H2O, the GOZCARDS product covers both stratosphere and mesosphere, and the same instruments as for HCl are used, along with Upper Atmosphere Research Satellite (UARS) MLS stratospheric H2O data (1991–1993). We display seasonal to decadal-type variability in H2O from 22 years of data. In the upper mesosphere, the anticorrelation between H2O and solar flux is now clearly visible over two full solar cycles. Lower-stratospheric tropical H2O has exhibited two periods of increasing values, followed by fairly sharp drops (the well-documented 2000–2001 decrease and a recent drop in 2011–2013). Tropical decadal variability peaks just above the tropopause. Between 1991 and 2013, both in the tropics and on a near-global basis, H2O has decreased by ~ 5–10 % in the lower stratosphere, but about a 10 % increase is observed in the upper stratosphere and lower mesosphere. However, such tendencies may not represent longer-term trends. For ozone, we used SAGE I, SAGE II, HALOE, UARS and Aura MLS, and ACE-FTS data to produce a merged record from late 1979 onward, using SAGE II as the primary reference. Unlike the 2 to 3 % increase in near-global column ozone after the late 1990s reported by some, GOZCARDS stratospheric column O3 values do not show a recent upturn of more than 0.5 to 1 %; long-term interannual column ozone variations from GOZCARDS are generally in very good agreement with interannual changes in merged total column ozone (Version 8.6) data from SBUV instruments. A brief mention is also made of other currently available, commonly formatted GOZCARDS satellite data records for stratospheric composition, namely those for N2O and HNO3.

A sudden stratospheric warming (SSW) in early January 2013 caused the Arctic polar vortex to split and temperatures to rapidly rise above the threshold for chlorine activation. However, ozone in the lower stratospheric polar vortex from late December 2012 through early February 2013 reached the lowest values on record for that time of year. Analysis of Aura Microwave Limb Sounder (MLS) trace gas measurements and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) polar stratospheric cloud (PSC) data shows that exceptional chemical ozone loss early in the 2012/13 Arctic winter resulted from a unique combination of meteorological conditions associated with the early-January 2013 SSW: unusually low temperatures in December 2012, offspring vortices within which air remained well isolated for nearly 1 month after the vortex split, and greater-than-usual vortex sunlight exposure throughout December 2012 and January 2013. Conditions in the two offspring vortices differed substantially, with the one overlying Canada having lower temperatures, lower nitric acid (HNO3), lower hydrogen chloride, more sunlight exposure/higher ClO in late January, and a later onset of chlorine deactivation than the one overlying Siberia. MLS HNO3 and CALIPSO data indicate that PSC activity in December 2012 was more extensive and persistent than at that time in any other Arctic winter in the past decade. Chlorine monoxide (ClO, measured by MLS) rose earlier than previously observed and was the largest on record through mid-January 2013. Enhanced vortex ClO persisted until mid-February despite the cessation of PSC activity when the SSW started. Vortex HNO3 remained depressed after PSCs had disappeared; passive transport calculations indicate vortex-averaged denitrification of about 4 parts per billion by volume. The estimated vortex-averaged chemical ozone loss, ~ 0.7–0.8 parts per million by volume near 500 K (~21 km), was the largest December/January loss in the MLS record from 2004/05 to 2014/15.

Sulfur dioxide (SO2) is an important atmospheric constituent, particularly in the aftermath of volcanic eruptions. These events can inject large amounts of SO2 into the lower stratosphere, where it is oxidised to form sulfate aerosols; these in turn have a significant effect on the climate. The MLS instrument on the Aura satellite has observed the SO2 mixing ratio in the upper troposphere and lower stratosphere from August 2004 to the present, during which time a number of volcanic eruptions have significantly affected those regions of the atmosphere. We describe the MLS SO2 data and how various volcanic events appear in the data. As the MLS SO2 data are currently not validated we take some initial steps towards their validation. First we establish the level of internal consistency between the three spectral regions in which MLS is sensitive to SO2. We compare SO2 column values calculated from MLS data to total column values reported by the OMI instrument. The agreement is good (within about 1 DU) in cases where the SO2 is clearly at altitudes above 147 hPa.

The interrelated geographic and temporal variability seen in more than seven years of tropical and subtropical upper tropospheric (215 hPa) ozone, carbon monoxide and cloud ice water content (IWC) observations by the Aura Microwave Limb Sounder (MLS) are presented. Observed ozone abundances and their variability (geographic and temporal) agree to within 10–15 ppbv with records from sonde observations. MLS complements these (and other) observations with global coverage and simultaneous measurements of related parameters. Previously-reported phenomena such as the ozone "wave one" feature are clearly seen in the MLS observations, as is a double peak in ozone abundance over tropical East Africa, with enhanced abundances in both May to June and September to November. While repeatable seasonal cycles are seen in many regions, they are often accompanied by significant interannual variability. Ozone seasonal cycles in the southern tropics and subtropics tend to be more distinct (i.e., annually repeatable) than in the northern. By contrast, carbon monoxide shows distinct seasonal cycles in many northern subtropical regions, notably from India to the Eastern Pacific. Deep convection (as indicated by large values of IWC) is typically associated with reductions in upper tropospheric ozone. Convection over polluted regions is seen to significantly enhance upper tropospheric carbon monoxide. While some regions show statistically significant correlations among ozone, carbon monoxide and IWC, simple correlations fall well short of accounting for the observed variability. The observed interrelated variations and metrics of annual and interannual variability described here represent a new resource for validation of atmospheric chemistry models.

The large bush fires which occurred in southeast Australia in February 2009 were unusually destructive. However, they were also unusual in the amounts of various combustion products which were injected directly into the stratosphere. We report the observations by the Microwave Limb Sounder (MLS) instrument on the Aura satellite of some of these combustion products. The highest quality observations are of CO; these clearly show a large region of enhanced mixing ratios to the north of New Zealand which remains in that region for about ten days before drifting westwards and finally dissipating over the Atlantic about a month after the fire. The region of enhanced CO ascends from the tropopause to 46 hPa during this period. Back trajectories run from the points where MLS observes enhanced CO pass close to the site of the fire. The MLS observations of CH3CN and HCN resemble those of CO except for their poorer vertical resolution and more limited vertical range. An apparent enhancement in ClO is also observed by MLS, but detailed analysis of the measured radiances reveals this feature to be a signature of CH3OH, which is not currently retrieved by the MLS data processing system. The fires of February 2009 are the only event of this type and magnitude in the 7-yr MLS record.

A method of classifying the upper tropospheric/lower stratospheric (UTLS) jets has been developed that allows satellite and aircraft trace gas data and meteorological fields to be efficiently mapped in a jet coordinate view. A detailed characterization of multiple tropopauses accompanies the jet characterization. Jet climatologies show the well-known high altitude subtropical and lower altitude polar jets in the upper troposphere, as well as a pattern of concentric polar and subtropical jets in the Southern Hemisphere, and shifts of the primary jet to high latitudes associated with blocking ridges in Northern Hemisphere winter. The jet-coordinate view segregates air masses differently than the commonly-used equivalent latitude (EqL) coordinate throughout the lowermost stratosphere and in the upper troposphere. Mapping O3 data from the Aura Microwave Limb Sounder (MLS) satellite and the Winter Storms aircraft datasets in jet coordinates thus emphasizes different aspects of the circulation compared to an EqL-coordinate framework: the jet coordinate reorders the data geometrically, thus highlighting the strong PV, tropopause height and trace gas gradients across the subtropical jet, whereas EqL is a dynamical coordinate that may blur these spatial relationships but provides information on irreversible transport. The jet coordinate view identifies the concentration of stratospheric ozone well below the tropopause in the region poleward of and below the jet core, as well as other transport features associated with the upper tropospheric jets. Using the jet information in EqL coordinates allows us to study trace gas distributions in regions of weak versus strong jets, and demonstrates weaker transport barriers in regions with less jet influence. MLS and Atmospheric Chemistry Experiment-Fourier Transform Spectrometer trace gas fields for spring 2008 in jet coordinates show very strong, closely correlated, PV, tropopause height and trace gas gradients across the jet, and evidence of intrusions of stratospheric air below the tropopause below and poleward of the subtropical jet; these features are consistent between instruments and among multiple trace gases. Our characterization of the jets is facilitating studies that will improve our understanding of upper tropospheric trace gas evolution.

Previous analyses of satellite and ground-based measurements of hydrogen chloride (HCl) and chlorine monoxide (ClO) have suggested that total inorganic chlorine in the upper stratosphere is on the decline. We create HCl and ClO time series using satellite data sets extended to November 2008, so that an update can be made on the long term evolution of these two species. We use the HALogen Occultation Experiment (HALOE) and the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) data for the HCl analysis, and the Odin Sub-Millimetre Radiometer (SMR) and the Aura Microwave Limb Sounder (Aura-MLS) measurements for the study of ClO. Altitudes between 35 and 45 km and two mid-latitude bands: 30° S–50° S and 30° N–50° N, for HCl, and 20° S–20° N for ClO and HCl are studied. ACE-FTS and HALOE HCl anomaly time series (with QBO and seasonal contributions removed) are combined to produce all instrument average time series, which show HCl to be reducing from peak 1997 values at a linear estimated rate of −5.1 % decade−1 in the Northern Hemisphere and −5.2 % decade−1 in the Southern Hemisphere, while the tropics show a linear trend of −5.8 % per decade (although we do not remove the QBO contribution there due to sparse data). Trend values are significantly different from a zero trend at the 2 sigma level. ClO is decreasing in the tropics by −7.1 % ± 7.8 % decade−1 based on measurements made from December 2001 to November 2008. The statistically significant downward trend found in HCl after 1997 and the apparent downward ClO trend since 2001 (although not statistically significant) confirm how effective the 1987 Montreal protocol objectives and its amendments have been in reducing the total amount of inorganic chlorine.

A space shuttle launch deposits 700 tonnes of water in the atmosphere. Some of this water is released into the upper mesosphere and lower thermosphere where it may be directly detected by a limb sounding satellite instrument. We report measurements of water vapour plumes from shuttle launches made by the Microwave Limb Sounder (MLS) on the Aura satellite. Approximately 50%–65% of shuttle launches are detected by MLS. The signal appears at a similar level across the upper 10 km of the MLS limb scan, suggesting that the bulk of the observed water is above the top of the scan. Only a small fraction at best of smaller launches (Ariane 5, Proton) are detected. We conclude that the sensitivity of MLS is only just great enough to detect a shuttle sized launch, but that a suitably designed instrument of the same general type could detect the exhausts from a large proportion of heavy-lift launches.

We use the GEOS-Chem chemistry-transport model (CTM) to interpret the spatial and temporal variations of tropical tropospheric CO observed by the Microwave Limb Sounder (MLS) and the Tropospheric Emission Spectrometer (TES). In so doing, we diagnose and evaluate transport in the GEOS-4 and GEOS-5 assimilated meteorological fields that drive the model, with a particular focus on vertical mixing at the end of the dry season when convection moves over the source regions. The results indicate that over South America, deep convection in both GEOS-4 and GEOS-5 decays at too low an altitude early in the wet season, and the source of CO from isoprene in the model (MEGAN v2.1) is too large, causing a lag in the model's seasonal maximum of CO compared to MLS CO in the upper troposphere (UT). TES and MLS data reveal problems with excessive transport of CO to the eastern equatorial Pacific and lofting in the ITCZ in August and September, particularly in GEOS-4. Over southern Africa, GEOS-4 and GEOS-5 simulations match the phase of the observed CO variation from the lower troposphere (LT) to the UT fairly well, although the magnitude of the seasonal maximum is underestimated considerably due to low emissions in the model. A sensitivity run with increased emissions leads to improved agreement with observed CO in the LT and middle troposphere (MT), but the amplitude of the seasonal variation is too high in the UT in GEOS-4. Difficulty in matching CO in the LT and UT implies there may be overly vigorous vertical mixing in GEOS-4 early in the wet season. Both simulations and observations show a time lag between the peak in fire emissions (July and August) and in CO (September and October). We argue that it is caused by the prevailing subsidence in the LT until convection moves south in September, as well as the low sensitivity of TES data in the LT over the African Plateau. The MLS data suggest that too much CO has been transported from fires in northern Africa to the UT in the model during the burning season, as does MOZAIC aircraft data, perhaps as a result of the combined influence of too strong Harmattan winds in the LT and too strong vertical mixing over the Gulf of Guinea in the model.

This paper presents an evaluation of a new linear parameterization valid for the troposphere and the stratosphere, based on a first order approximation of the carbon monoxide (CO) continuity equation. This linear scheme (hereinafter noted LINCO) has been implemented in the 3-D Chemical Transport Model (CTM) MOCAGE (MOdèle de Chimie Atmospherique Grande Echelle). First, a one and a half years of LINCO simulation has been compared to output obtained from a detailed chemical scheme output. The mean differences between both schemes are about ±25 ppbv (part per billion by volume) or 15% in the troposphere and ±10 ppbv or 100% in the stratosphere. Second, LINCO has been compared to diverse observations from satellite instruments covering the troposphere (Measurements Of Pollution In The Troposphere: MOPITT) and the stratosphere (Microwave Limb Sounder: MLS) and also from aircraft (Measurements of ozone and water vapour by Airbus in-service aircraft: MOZAIC programme) mostly flying in the upper troposphere and lower stratosphere (UTLS). In the troposphere, the LINCO seasonal variations as well as the vertical and horizontal distributions are quite close to MOPITT CO observations. However, a bias of ~−40 ppbv is observed at 700 Pa between LINCO and MOPITT. In the stratosphere, MLS and LINCO present similar large-scale patterns, except over the poles where the CO concentration is underestimated by the model. In the UTLS, LINCO presents small biases less than 2% compared to independent MOZAIC profiles. Third, we assimilated MOPITT CO using a variational 3D-FGAT (First Guess at Appropriate Time) method in conjunction with MOCAGE for a long run of one and a half years. The data assimilation greatly improves the vertical CO distribution in the troposphere from 700 to 350 hPa compared to independent MOZAIC profiles. At 146 hPa, the assimilated CO distribution is also improved compared to MLS observations by reducing the bias up to a factor of 2 in the tropics. This study confirms that the linear scheme is able to simulate reasonably well the CO distribution in the troposphere and in the lower stratosphere. Therefore, the low computing cost of the linear scheme opens new perspectives to make free runs and CO data assimilation runs at high resolution and over periods of several years.

An unusually strong and prolonged stratospheric sudden warming (SSW) in January 2006 was the first major SSW for which globally distributed long-lived trace gas data are available covering the upper troposphere through the lower mesosphere. We use Aura Microwave Limb Sounder (MLS), Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS) data, the SLIMCAT Chemistry Transport Model (CTM), and assimilated meteorological analyses to provide a comprehensive picture of transport during this event. The upper tropospheric ridge that triggered the SSW was associated with an elevated tropopause and layering in trace gas profiles in conjunction with stratospheric and tropospheric intrusions. Anomalous poleward transport (with corresponding quasi-isentropic troposphere-to-stratosphere exchange at the lowest levels studied) in the region over the ridge extended well into the lower stratosphere. In the middle and upper stratosphere, the breakdown of the polar vortex transport barrier was seen in a signature of rapid, widespread mixing in trace gases, including CO, H2O, CH4 and N2O. The vortex broke down slightly later and more slowly in the lower than in the middle stratosphere. In the middle and lower stratosphere, small remnants with trace gas values characteristic of the pre-SSW vortex lingered through the weak and slow recovery of the vortex. The upper stratospheric vortex quickly reformed, and, as enhanced diabatic descent set in, CO descended into this strong vortex, echoing the fall vortex development. Trace gas evolution in the SLIMCAT CTM agrees well with that in the satellite trace gas data from the upper troposphere through the middle stratosphere. In the upper stratosphere and lower mesosphere, the SLIMCAT simulation does not capture the strong descent of mesospheric CO and H2O values into the reformed vortex; this poor CTM performance in the upper stratosphere and lower mesosphere results primarily from biases in the diabatic descent in assimilated analyses.

During several periods since 2005 the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat has performed observations dedicated to the region of the upper troposphere/lower stratosphere (UTLS). For the duration of November/December 2005 global distributions of temperature and several trace gases from MIPAS UTLS-1 mode measurements have been retrieved using the IMK/IAA (Institut für Meteorologie und Klimaforschung/Instituto de Astrofísica de Andalucía) scientific processor. In the UTLS region a vertical resolution of 3 km for temperaure, 3 to 4 km for H2O, 2.5 to 3 km for O3, 3.5 km for HNO3 and 3.5 to 2.5 km for N2O has been achieved. The retrieved temperature, H2O, O3, HNO3, N2O, and relative humidity over ice are intercompared with the Microwave Limb Sounder (MLS/Aura) v2.2 data in the pressure range 316 to 0.68 hPa, 316 to 0.68 hPa, 215 to 0.68 hPa, 215 to 3.16 hPa, 100 to 1 hPa and 316 to 10 hPa, respectively. In general, MIPAS and MLS temperatures are biased within ±4 K over the whole pressure and latitude range. Systematic, latitude-independent differences of −2 to −4 K (MIPAS-MLS) at 121 hPa are explained by previously observed biases in the MLS v2.2 temperature retrievals. Temperature differences of −4 K up to 12 K above 10.0 hPa are present both in MIPAS and MLS with respect to ECMWF (European Centre for Medium-Range Weather Forecasts) and are likely due to deficiencies of the ECMWF analysis data. MIPAS and MLS stratospheric volume mixing ratios (vmr) of H2O are biased within ±1 ppmv, with indication of oscillations between 146 and 26 hPa in the MLS dataset. Tropical upper tropospheric values of relative humidity over ice measured by the two instruments differ by ±20% in the pressure range ~146 to 68 hPa. These differences are mainly caused by the MLS temperature biases. Ozone mixing ratios agree within 0.5 ppmv (10 to 20%) between 68 and 14 hPa. At pressures smaller than 10 hPa, MIPAS O3 vmr are higher than MLS by an average of 0.5 ppmv (10%). General agreement between MIPAS and MLS HNO3 is within the range of −1.0 (−10%) to 1.0 ppbv (20%). MIPAS HNO3 is 1.0 ppbv (10%) higher compared to MLS between 46 hPa and 10 hPa over the Northern Hemisphere. Over the tropics at 31.6 hPa MLS shows a low bias of more than 1 ppbv (>50%). In general, MIPAS and MLS N2O vmr agree within 20 to 40 ppbv (20 to 40%). Differences in the range between 100 to 21 hPa are attributed to a known 20% positive bias in MIPAS N2O data.

We have studied the effects of the 2006 El Niño on tropospheric O3 and CO at tropical and sub-tropical latitudes measured from the OMI and MLS instruments on the Aura satellite. The 2006 El Niño-induced drought caused forest fires (largely set to clear land) to burn out of control during October and November in the Indonesian region. The effects of these fires are clearly seen in the enhancement of CO concentration measured from the MLS instrument. We have used a global model of atmospheric chemistry and transport (GMI CTM) to quantify the relative importance of biomass burning and large scale transport in producing observed changes in tropospheric O3 and CO. The model results show that during October and November biomass burning and meteorological changes contributed almost equally to the observed increase in tropospheric O3 in the Indonesian region. The biomass component was 4–6 DU but it was limited to the Indonesian region where the fires were most intense. The dynamical component was 4–8 DU but it covered a much larger area in the Indian Ocean extending from South East Asia in the north to western Australia in the south. By December 2006, the effect of biomass burning was reduced to zero and the observed changes in tropospheric O3 were mostly due to dynamical effects. The model results show an increase of 2–3% in the global burden of tropospheric ozone. In comparison, the global burden of CO increased by 8–12%.

Estimates of the radiative forcing due to anthropogenically-produced tropospheric O3 are derived primarily from models. Here, we use tropospheric ozone and cloud data from several instruments in the A-train constellation of satellites as well as information from the GEOS-5 Data Assimilation System to accurately estimate the radiative effect of tropospheric O3 for January and July 2005. Since we cannot distinguish between natural and anthropogenic sources with the satellite data, our derived radiative effect reflects the unadjusted (instantaneous) effect of the total tropospheric O3 rather than the anthropogenic component. We improve upon previous estimates of tropospheric ozone mixing ratios from a residual approach using the NASA Earth Observing System (EOS) Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) by incorporating cloud pressure information from OMI. We focus specifically on the magnitude and spatial structure of the cloud effect on both the short- and long-wave radiative budget. The estimates presented here can be used to evaluate the various aspects of model-generated radiative forcing. For example, our derived cloud impact is to reduce the radiative effect of tropospheric ozone by ~16%. This is centered within the published range of model-produced cloud effect on unadjusted ozone radiative forcing.

This paper presents extensive {bias determination} 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. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from nearly 20 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 average values of the mean relative differences are nearly all within +1 to +8%. At higher altitudes (45–60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments, with mean relative differences of up to +40% (about +20% on average). For the ACE-MAESTRO version 1.2 ozone data product, mean relative differences are within ±10% (average values within ±6%) between 18 and 40 km for both the sunrise and sunset measurements. At higher altitudes (~35–55 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 (with mean relative differences down to −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS, indicating a large positive bias (mean relative differences within +10 to +30%) in the 45–55 km altitude range. In contrast, there is no significant systematic difference in bias found for the ACE-FTS sunrise and sunset measurements.

Mechanisms for transporting and dehydrating air across the tropical tropopause layer (TTL) are investigated with a conceptual two dimensional (2-D) model. The 2-D TTL model combines the Holton and Gettelman cold trap dehydration mechanism (Holton and Gettelman, 2001) with the two column convection model of Folkins and Martin (2005). We investigate 3 possible transport scenarios through the TTL: 1) slow uniform ascent across the level of zero radiative heating without direct convective mixing, 2) convective mixing of H2O vapor at 100% relative humidity with respect to ice (RHi) with no ice retention, and 3) convective mixing of extremely subsaturated air (100% RHi following the moist adiabatic temperature above the level of neutral buoyancy) with sufficient ice retention such that total H2O is 100%RHi. The three mechanisms produce similar seasonal cycles for H2O that are in good quantitative agreement with the Aura Microwave Limb Sounder (MLS) measurements. We use Aura MLS measurement of CO and Atmospheric Chemistry Experiment-Fourier Transform Spectrometer measurement of HDO to distinguish among the transport mechanisms. Model comparisons with the observations support the view that H2O is predominantly controlled by regions having the lowest cold point tropopause temperature but the trace species CO and HDO support the convective mixing of dry air and lofted ice. The model provides some insight into the processes affecting the long term trends observed in stratospheric H2O.

The transport pathways of carbon monoxide (CO) in the African Upper Troposphere (UT) during the West African Monsoon (WAM) is investigated through the assimilation of CO observations by the Aura Microwave Limb Sounder (MLS) in the MOCAGE Chemistry Transport Model (CTM). The assimilation setup, based on a 3-D First Guess at Assimilation Time (3-D-FGAT) variational method is described. Comparisons between the assimilated CO fields and in situ airborne observations from the MOZAIC program between Europe and both Southern Africa and Southeast Asia show an overall good agreement around the lowermost pressure level sampled by MLS (~215 hPa). The 4-D assimilated fields averaged over the month of July 2006 have been used to determine the main dynamical processes responsible for the transport of CO in the African UT. The studied period corresponds to the second AMMA (African Monsoon Multidisciplinary Analyses) aircraft campaign. At 220 hPa, the CO distribution is characterized by a latitudinal maximum around 5° N mostly driven by convective uplift of air masses impacted by biomass burning from Southern Africa, uplifted within the WAM region and vented predominantly southward by the upper branch of the winter hemisphere Hadley cell. Above 150 hPa, the African CO distribution is characterized by a broad maximum over northern Africa. This maximum is mostly controlled by the large scale UT circulation driven by the Asian Summer Monsoon (ASM) and characterized by the Asian Monsoon Anticyclone (AMA) centered at 30° N and the Tropical Easterly Jet (TEJ) on the southern flank of the anticyclone. Asian pollution uplifted to the UT over large region of Southeast Asia is trapped within the AMA and transported by the anticyclonic circulation over Northeast Africa. South of the AMA, the TEJ is responsible for the tranport of CO-enriched air masses from India and Southeast Asia over Africa. Using the high time resolution provided by the 4-D assimilated fields, we give evidence that the variability of the African CO distribution above 150 hPa and north of the WAM region is mainly driven by the synoptic dynamical variability of both the AMA and the TEJ.

The Atmospheric Chemistry Experiment (ACE) mission was launched in August 2003 to sound the atmosphere by solar occultation. Carbon monoxide (CO), a good tracer of pollution plumes and atmospheric dynamics, is one of the key species provided by the primary instrument, the ACE-Fourier Transform Spectrometer (ACE-FTS). This instrument performs measurements in both the CO 1-0 and 2-0 ro-vibrational bands, from which vertically resolved CO concentration profiles are retrieved, from the mid-troposphere to the thermosphere. This paper presents an updated description of the ACE-FTS version 2.2 CO data product, along with a comprehensive validation of these profiles using available observations (February 2004 to December 2006). We have compared the CO partial columns with ground-based measurements using Fourier transform infrared spectroscopy and millimeter wave radiometry, and the volume mixing ratio profiles with airborne (both high-altitude balloon flight and airplane) observations. CO satellite observations provided by nadir-looking instruments (MOPITT and TES) as well as limb-viewing remote sensors (MIPAS, SMR and MLS) were also compared with the ACE-FTS CO products. We show that the ACE-FTS measurements provide CO profiles with small retrieval errors (better than 5% from the upper troposphere to 40 km, and better than 10% above). These observations agree well with the correlative measurements, considering the rather loose coincidence criteria in some cases. Based on the validation exercise we assess the following uncertainties to the ACE-FTS measurement data: better than 15% in the upper troposphere (8–12 km), than 30% in the lower stratosphere (12–30 km), and than 25% from 30 to 100 km.

The first three Arctic winters of the ACE mission represented two extremes of winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns were conducted at Eureka (80° N, 86° W) during each of these winters. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), and Aura Microwave Limb Sounder (MLS), along with meteorological analyses and Eureka lidar temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport, and to provide a context for interpretation of ACE-FTS and validation campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, near 75 km. ACE measurements covered both vortex and extra-vortex conditions in each winter, except in late-February through mid-March 2004 and 2006, when the strong, pole-centered vortex that reformed after the SSWs resulted in ACE sampling only inside the vortex in the middle through upper stratosphere. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with lidar data up to 50–60 km, and ACE-FTS, MLS and SABER show good agreement in high-latitude temperatures throughout the winters. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex in late January through March 2006 compared to that in 2005.