Search

This work uses multispectral measurements of vertically resolved aerosol extinction coefficients from the Stratospheric Aerosol and Gas Experiment (SAGE) III on the International Space Station (ISS) to demonstrate how the use of the Ångström exponent for interpolation of aerosol data between two different wavelengths creates a bias. An empirical relationship is derived between the magnitude of this bias and the Ångström exponent at several different SAGE wavelengths. This relationship can thus be used as a correction factor for other studies, such as multi-instrument intercomparisons or merging, that wish to convert aerosol data from one wavelength to another using the Ångström exponent and is applicable to all stratospheric non-cloud aerosol except highly aged particles that are evaporating at altitudes above the Junge layer.

Using a common analysis approach for data sets produced by the Stratospheric Aerosol and Gas Experiment instruments SAGE II and SAGE III/ISS, we identify 13 likely smoke events based on enhancements in the aerosol extinction coefficient. Nine of these are sufficiently large compared to ambient aerosol levels to compute mean mid-latitude 1020 nm optical depth enhancements that range from 0.0005 to 0.011. We also note that, for large events, the 525 to 1020 nm aerosol extinction coefficient ratio asymptotes at a high extinction coefficient to values between 2 and 3, suggesting that the aerosol radius is relatively small (< 0.3 µm) and relatively consistent from event to event. Most of these events are primarily confined to the lower stratosphere and rarely can be observed above 20 km. We also infer an increase in the frequency of smoke events between the SAGE II (1984–1991, 1996–2005) and SAGE III/ISS (2017-present) periods by almost a factor of 2 and also note that the two largest events occur in the latter data set. However, given the low frequencies overall, we are not confident that the differences can be attributed to changes between the two periods. We also attempt to disentangle the mixing of aerosol in the Northern Hemisphere summer of 1991 from a pyrocumulus event (Baie-Comeau, Quebec) and Mt. Pinatubo and conclude that, while there is evidence for smoke in the lower stratosphere, virtually all of the enhanced aerosol observations in the northern mid-latitudes in the summer of 1991 are associated with the Mt. Pinatubo eruption.

The stratospheric aerosol layer plays an important role in the radiative balance of Earth primarily through scattering of solar radiation. The magnitude of this effect depends critically on the size distribution of the aerosol. The aerosol layer is in large part fed by volcanic eruptions strong enough to inject gaseous sulfur species into the stratosphere. The evolution of the stratospheric aerosol size after volcanic eruptions is currently one of the biggest uncertainties in stratospheric aerosol science. We retrieved aerosol particle size information from satellite solar occultation measurements from the Stratospheric Aerosol and Gas Experiment III mounted on the International Space Station (SAGE III/ISS) using a robust spectral method. We show that, surprisingly, some volcanic eruptions can lead to a decrease in average aerosol size, like the 2018 Ambae and the 2021 La Soufrière eruptions. In 2019 an intriguing contrast is observed, where the Raikoke eruption (48∘ N, 153∘ E) in 2019 led to the more expected stratospheric aerosol size increase, while the Ulawun eruptions (5∘ S, 151∘ E), which followed shortly after, again resulted in a reduction in the values of the median radius and absolute distribution width in the lowermost stratosphere. In addition, the Raikoke and Ulawun eruptions were simulated with the aerosol climate model MAECHAM5-HAM. In these model runs, the evolution of the extinction coefficient as well as of the effective radius could be reproduced well for the first 3 months of volcanic activity. However, the long lifetime of the very small aerosol sizes of many months observed in the satellite retrieval data could not be reproduced.

In this work, a novel approach for the determination of the particle size distribution (PSD) parameters of stratospheric sulfate aerosols is presented. For this, ratios of extinction coefficients obtained from SAGE III/ISS (Stratospheric Aerosol and Gas Experiment III on the International Space Station) solar occultation measurements at 449, 756 and 1544 nm were used to retrieve the mode width and median radius of a size distribution assumed to be monomodal lognormal. The estimated errors at the peak of the stratospheric aerosol layer, on average, lie between 20 % and 25 % for the median radius and 5 % and 7 % for the mode width. The results are consistent in magnitude with other retrieval results from the literature, but a robust comparison is difficult, mainly because of differences in temporal and spatial coverage. Other quantities like number density and effective radius were also calculated. A major advantage of the described method over other retrieval techniques is that both the median radius and the mode width can be retrieved simultaneously, without having to assume one of them. This is possible due to the broad wavelength spectrum covered by the SAGE III/ISS measurements. Also, the presented method – being based on the analysis of three wavelengths – allows unique solutions for the retrieval of PSD parameters for almost all of the observed extinction spectra, which is not the case when using only two spectral channels. In addition, the extinction coefficients from SAGE III/ISS solar occultation measurements, on which the retrieval is based, are calculated without a priori assumptions about the PSD. For those reasons, the data produced with the presented retrieval technique may be a valuable contribution for a better understanding of the variability of stratospheric aerosol size distributions, e.g. after volcanic eruptions. While this study focuses on describing the retrieval method, and a future study will discuss the PSD parameter data set produced in depth, some exemplary results for background conditions in June 2017 are shown.

An analysis of multiwavelength stratospheric aerosol extinction coefficient data from the Stratospheric Aerosol and Gas Experiment II and III/ISS instruments is used to demonstrate a coherent relationship between the perturbation in extinction coefficient in an eruption's main aerosol layer and the wavelength dependence of that perturbation. This relationship spans multiple orders of magnitude in the aerosol extinction coefficient of stratospheric impact of volcanic events. The relationship is measurement-based and does not rely on assumptions about the aerosol size distribution. We note limitations on this analysis including that the presence of significant amounts of ash in the main sulfuric acid aerosol layer and other factors may significantly modulate these results. Despite these limitations, the findings suggest an avenue for improving aerosol extinction coefficient measurements from single-channel observations such as the Optical Spectrograph and Infrared Imager System as they rely on a prior assumptions about particle size. They may also represent a distinct avenue for the comparison of observations with interactive aerosol models used in global climate models and Earth system models.

A key limitation of volcanic forcing datasets for the Pinatubo period is the large uncertainty that remains with respect to the extent of the optical depth of the Pinatubo aerosol cloud in the first year after the eruption, the saturation of the SAGE-II instrument restricting it to only be able to measure the upper part of the aerosol cloud in the tropics. Here we report the recovery of stratospheric aerosol measurements from two shipborne lidars, both of which measured the tropical reservoir of volcanic aerosol produced by the June 1991 Mount Pinatubo eruption. The lidars were on board two Soviet vessels, each ship crossing the Atlantic, their measurement datasets providing unique observational transects of the Pinatubo cloud across the tropics from Europe to the Caribbean (∼ 40 to 8∘ N) from July to September 1991 (the Professor Zubov ship) and from Europe to south of the Equator (∼ 40∘ N to 8∘ S) between January and February 1992 (the Professor Vize ship). Our philosophy with the data recovery is to follow the same algorithms and parameters that appear in the two peer-reviewed articles that presented these datasets in the same issue of GRL in 1993, and here we provide all 48 lidar soundings made from the Professor Zubov and 11 of the 20 conducted from the Professor Vize, ensuring we have reproduced the aerosol backscatter and extinction values in the figures of those two papers. These original approaches used thermodynamic properties from the CIRA-86 standard atmosphere to derive the molecular backscattering, vertically and temporally constant values applied for the aerosol backscatter-to-extinction ratio, and the correction factor of the aerosol backscatter wavelength dependence. We demonstrate this initial validation of the recovered stratospheric aerosol extinction profiles, providing full details of each dataset in this paper's Supplement S1, the original profiles of backscatter ratio, and the calculated profiles of aerosol backscatter and extinction. We anticipate these datasets will provide potentially important new observational case studies for modelling analyses, including a 1-week series of consecutive soundings (in September 1991) at the same location showing the progression of the entrainment of part of the Pinatubo plume into the upper troposphere and the formation of an associated cirrus cloud. The Zubov lidar dataset illustrates how the tropically confined Pinatubo aerosol cloud transformed from a highly heterogeneous vertical structure in August 1991, maximum aerosol extinction values around 19 km for the lower layer and 23–24 for the upper layer, to a more homogeneous and deeper reservoir of volcanic aerosol in September 1991. We encourage modelling groups to consider new analyses of the Pinatubo cloud, comparing the recovered datasets, with the potential to increase our understanding of the evolution of the Pinatubo aerosol cloud and its effects. Data described in this work are available at https://doi.org/10.1594/PANGAEA.912770 (Antuña-Marrero et al., 2020).

A robust stratospheric aerosol climate data record enables the depiction of the radiative forcing of this highly variable component of climate. In addition to the radiative forcing, stratospheric aerosol also plays a key role in the chemical processes leading to ozone depletion. Therefore, stratospheric aerosol is one of the crucial parameters in understanding climate change in the past and potential changes in the future. As a part of Stratospheric-tropospheric Processes and their Role in Climate (SPARC) Stratospheric Sulfur and its Role in Climate (SSiRC) activity, the Global Space-based Stratospheric Aerosol Climatology (GloSSAC) was created (Thomason et al., 2018) to support the World Climate Research Programme's (WCRP) Coupled Model Intercomparison Project Phase 6 (CMIP6) (Eyring et al., 2016). This data set is a follow-on to one created as a part of SPARC's Assessment of Stratospheric Aerosol Properties (ASAP) activity (SPARC, 2006) and a data created for the Chemistry-Climate Model Initiative (CCMI) in 2012 (Eyring and Lamarque, 2012). Herein, we discuss changes to the original release version including those as a part of v1.1 that was released in September 2018 that primarily corrects an error in the conversion of Cryogenic Limb Array Etalon Spectrometer (CLAES) data to Stratospheric Aerosol and Gas Experiment (SAGE) II wavelengths, as well as the new release, v2.0. Version 2.0 is focused on improving the post-SAGE II era (after 2005) with the goal of mitigating elevated aerosol extinction in the lower stratosphere at mid- and high latitudes noted in v1.0 as noted in Thomason et al. (2018). Changes include the use of version 7.0 of the Optical Spectrograph and InfraRed Imaging System (OSIRIS), the recently released Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar Level 3 stratospheric aerosol profile monthly product and the new addition of SAGE III/ISS. Here, we use an observed relationship between (i) OSIRIS extinction at 750 nm and (ii) SAGE II and SAGE III/ISS extinction at 525 nm to derive an altitude–latitude-based monthly climatology of Ångström exponent to compute OSIRIS extinction at 525 nm, resulting in a better agreement between OSIRIS and SAGE measurements. We employ a similar approach to convert OSIRIS 750 nm extinction to 1020 nm extinction for the post-SAGE II period. Additionally, we incorporate the recently released standard CALIPSO stratospheric aerosol profile monthly product into GloSSAC with an improved conversion technique of the 532 nm backscatter coefficient to extinction using an observed relationship between OSIRIS 525 nm extinction and CALIPSO 532 nm backscatter. SAGE III/ISS data are also incorporated in GloSSAC to extend the climatology to the present and to test the approach used to correct OSIRIS/CALIPSO data. The GloSSAC v2.0 netCDF file is accessible at https://doi.org/10.5067/glossac-l3-v2.0 (Thomason, 2020).

High-quality satellite-based measurements are crucial to the assessment of global stratospheric composition change. The Stratospheric Aerosol and Gas Experiment II (SAGE II) provides the longest, continuous data set of vertically resolved ozone and aerosol extinction coefficients to date and therefore remains a cornerstone of understanding and detecting long-term ozone variability and trends in the stratosphere. Despite its stability, SAGE II measurements must be screened for outliers that are a result of excessive aerosol emitted into the atmosphere and that degrade inferences of change. Current methods for SAGE II ozone measurement quality assurance consist of multiple ad hoc and sometimes conflicting rules, leading to too much valuable data being removed or outliers being missed. In this work, the SAGE II ozone data set version 7.00 is used to develop and present a new set of screening recommendations and to compare the output to the screening recommendations currently used. Applying current recommendations to SAGE II ozone leads to unexpected features, such as removing ozone values around zero if the relative error is used as a screening criterion, leading to biases in monthly mean zonal mean ozone concentrations. Most of these current recommendations were developed based on “visual inspection”, leading to inconsistent rules that might not be applicable at every altitude and latitude. Here, a set of new screening recommendations is presented that take into account the knowledge of how the measurements were made. The number of screening recommendations is reduced to three, which mainly remove ozone values that are affected by high aerosol loading and are therefore not reliable measurements. More data remain when applying these new recommendations compared to the rules that are currently being used, leading to more data being available for scientific studies. The SAGE II ozone data set used here is publicly available at https://doi.org/10.5281/zenodo.3710518 (Kremser et al., 2020). The complete SAGE II version 7.00 data set, which includes other variables in addition to ozone, is available at https://eosweb.larc.nasa.gov/project/sage2/sage2_v7_table (last access: December 2019), https://doi.org/10.5067/ERBS/SAGEII/SOLAR_BINARY_L2-V7.0 (SAGE II Science Team, 2012; Damadeo et al., 2013).

We show that a fire plume injected into the lower stratosphere at high northern latitudes during the Canadian wildfire event in August 2017 partly reached the tropics. The transport to the tropics was mediated by the anticyclonic flow of the Asian monsoon circulation. The fire plume reached the Asian monsoon area in late August/early September, when the Asian monsoon anticyclone (AMA) was still in place. While there is no evidence of mixing into the center of the AMA, we show that a substantial part of the fire plume is entrained into the anticyclonic flow at the AMA edge and is transported from the extratropics to the tropics, and possibly the Southern Hemisphere particularly following the north–south flow on the eastern side of the AMA. In the tropics the fire plume is lifted by ∼5 km in 7 months. Inside the AMA we find evidence of the Asian tropopause aerosol layer (ATAL) in August, doubling background aerosol conditions with a calculated top of the atmosphere shortwave radiative forcing of −0.05 W m−2. The regional climate impact of the fire signal in the wider Asian monsoon area in September exceeds the impact of the ATAL by a factor of 2–4 and compares to that of a plume coming from an advected moderate volcanic eruption. The stratospheric, trans-continental transport of this plume to the tropics and the related regional climate impact point to the importance of long-range dynamical interconnections of pollution sources.

We describe the construction of a continuous 38-year record of stratospheric aerosol optical properties. The Global Space-based Stratospheric Aerosol Climatology, or GloSSAC, provided the input data to the construction of the Climate Model Intercomparison Project stratospheric aerosol forcing data set (1979–2014) and we have extended it through 2016 following an identical process. GloSSAC focuses on the Stratospheric Aerosol and Gas Experiment (SAGE) series of instruments through mid-2005, and on the Optical Spectrograph and InfraRed Imager System (OSIRIS) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) data thereafter. We also use data from other space instruments and from ground-based, air, and balloon borne instruments to fill in key gaps in the data set. The end result is a global and gap-free data set focused on aerosol extinction coefficient at 525 and 1020 nm and other parameters on an "as available" basis. For the primary data sets, we developed a new method for filling the post-Pinatubo eruption data gap for 1991–1993 based on data from the Cryogenic Limb Array Etalon Spectrometer. In addition, we developed a new method for populating wintertime high latitudes during the SAGE period employing a latitude-equivalent latitude conversion process that greatly improves the depiction of aerosol at high latitudes compared to earlier similar efforts. We report data in the troposphere only when and where it is available. This is primarily during the SAGE II period except for the most enhanced part of the Pinatubo period. It is likely that the upper troposphere during Pinatubo was greatly enhanced over non-volcanic periods and that domain remains substantially under-characterized. We note that aerosol levels during the OSIRIS/CALIPSO period in the lower stratosphere at mid- and high latitudes is routinely higher than what we observed during the SAGE II period. While this period had nearly continuous low-level volcanic activity, it is possible that the enhancement in part reflects deficiencies in the data set. We also expended substantial effort to quality assess the data set and the product is by far the best we have produced. GloSSAC version 1.0 is available in netCDF format at the NASA Atmospheric Data Center at https://eosweb.larc.nasa.gov/. GloSSAC users should cite this paper and the data set DOI (https://doi.org/10.5067/GloSSAC-L3-V1.0).

Stratospheric aerosol extinction profiles have been retrieved from SCIAMACHY/Envisat measurements of limb-scattered solar radiation. The retrieval is an improved version of an algorithm presented earlier. The retrieved aerosol extinction profiles are compared to co-located aerosol profile measurements from the SAGE II solar occultation instrument at a wavelength of 525 nm. Comparisons were carried out with two versions of the SAGE II data set (version 6.2 and the new version 7.0). In a global average sense the SCIAMACHY and the SAGE II version 7.0 extinction profiles agree to within about 10 % for altitudes above 15 km. Larger relative differences (up to 40 %) are observed at specific latitudes and altitudes. We also find differences between the two SAGE II data versions of up to 40 % for specific latitudes and altitudes, consistent with earlier reports. Sample results on the latitudinal and temporal variability of stratospheric aerosol extinction and optical depth during the SCIAMACHY mission period are presented. The results confirm earlier reports that a series of volcanic eruptions is responsible for the increase in stratospheric aerosol optical depth from 2002 to 2012. Above about an altitude of 28 km, volcanic eruptions are found to have negligible impact in the period 2002–2012.

This paper details a new method of regression for sparsely sampled data sets for use with time-series analysis, in particular the Stratospheric Aerosol and Gas Experiment (SAGE) II ozone data set. Non-uniform spatial, temporal, and diurnal sampling present in the data set result in biased values for the long-term trend if not accounted for. This new method is performed close to the native resolution of measurements and is a simultaneous temporal and spatial analysis that accounts for potential diurnal ozone variation. Results show biases, introduced by the way data are prepared for use with traditional methods, can be as high as 10%. Derived long-term changes show declines in ozone similar to other studies but very different trends in the presumed recovery period, with differences up to 2% per decade. The regression model allows for a variable turnaround time and reveals a hemispheric asymmetry in derived trends in the middle to upper stratosphere. Similar methodology is also applied to SAGE II aerosol optical depth data to create a new volcanic proxy that covers the SAGE II mission period. Ultimately this technique may be extensible towards the inclusion of multiple data sets without the need for homogenization.

We use a stratosphere–troposphere composition–climate model with interactive sulfur chemistry and aerosol microphysics, to investigate the effect of the 1991 Mount Pinatubo eruption on stratospheric aerosol properties. Satellite measurements indicate that shortly after the eruption, between 14 and 23 Tg of SO2 (7 to 11.5 Tg of sulfur) was present in the tropical stratosphere. Best estimates of the peak global stratospheric aerosol burden are in the range 19 to 26 Tg, or 3.7 to 6.7 Tg of sulfur assuming a composition of between 59 and 77 % H2SO4. In light of this large uncertainty range, we performed two main simulations with 10 and 20 Tg of SO2 injected into the tropical lower stratosphere. Simulated stratospheric aerosol properties through the 1991 to 1995 period are compared against a range of available satellite and in situ measurements. Stratospheric aerosol optical depth (sAOD) and effective radius from both simulations show good qualitative agreement with the observations, with the timing of peak sAOD and decay timescale matching well with the observations in the tropics and mid-latitudes. However, injecting 20 Tg gives a factor of 2 too high stratospheric aerosol mass burden compared to the satellite data, with consequent strong high biases in simulated sAOD and surface area density, with the 10 Tg injection in much better agreement. Our model cannot explain the large fraction of the injected sulfur that the satellite-derived SO2 and aerosol burdens indicate was removed within the first few months after the eruption. We suggest that either there is an additional alternative loss pathway for the SO2 not included in our model (e.g. via accommodation into ash or ice in the volcanic cloud) or that a larger proportion of the injected sulfur was removed via cross-tropopause transport than in our simulations. We also critically evaluate the simulated evolution of the particle size distribution, comparing in detail to balloon-borne optical particle counter (OPC) measurements from Laramie, Wyoming, USA (41° N). Overall, the model captures remarkably well the complex variations in particle concentration profiles across the different OPC size channels. However, for the 19 to 27 km injection height-range used here, both runs have a modest high bias in the lowermost stratosphere for the finest particles (radii less than 250 nm), and the decay timescale is longer in the model for these particles, with a much later return to background conditions. Also, whereas the 10 Tg run compared best to the satellite measurements, a significant low bias is apparent in the coarser size channels in the volcanically perturbed lower stratosphere. Overall, our results suggest that, with appropriate calibration, aerosol microphysics models are capable of capturing the observed variation in particle size distribution in the stratosphere across both volcanically perturbed and quiescent conditions. Furthermore, additional sensitivity simulations suggest that predictions with the models are robust to uncertainties in sub-grid particle formation and nucleation rates in the stratosphere.

In terms of atmospheric impact, the volcanic eruption of Mt. Pinatubo (1991) is the best characterized large eruption on record. We investigate here the model-derived stratospheric warming following the Pinatubo eruption as derived from SAGE II extinction data including recent improvements in the processing algorithm. This method, termed SAGE_4λ, makes use of the four wavelengths (385, 452, 525 and 1024 nm) of the SAGE II data when available, and uses a data-filling procedure in the opacity-induced "gap" regions. Using SAGE_4λ, we derived aerosol size distributions that properly reproduce extinction coefficients also at much longer wavelengths. This provides a good basis for calculating the absorption of terrestrial infrared radiation and the resulting stratospheric heating. However, we also show that the use of this data set in a global chemistry–climate model (CCM) still leads to stronger aerosol-induced stratospheric heating than observed, with temperatures partly even higher than the already too high values found by many models in recent general circulation model (GCM) and CCM intercomparisons. This suggests that the overestimation of the stratospheric warming after the Pinatubo eruption may not be ascribed to an insufficient observational database but instead to using outdated data sets, to deficiencies in the implementation of the forcing data, or to radiative or dynamical model artifacts. Conversely, the SAGE_4λ approach reduces the infrared absorption in the tropical tropopause region, resulting in a significantly better agreement with the post-volcanic temperature record at these altitudes.

We describe the challenges associated with the interpretation of extinction coefficient measurements by the Stratospheric Aerosol and Gas Experiment (SAGE II) in the presence of clouds. In particular, we have found that tropospheric aerosol analyses are highly dependent on a robust method for identifying when clouds affect the measured extinction coefficient. Herein, we describe an improved cloud identification method that appears to capture cloud/aerosol events more effectively than early methods. In addition, we summarize additional challenges to observing the Asian Tropopause Aerosol Layer (ATAL) using SAGE II observations. Using this new approach, we perform analyses of the upper troposphere, focusing on periods in which the UTLS (upper troposphere/lower stratosphere) is relatively free of volcanic material (1989–1990 and after 1996). Of particular interest is the Asian monsoon anticyclone where CALIPSO (Cloud-Aerosol Lidar Pathfinder Satellite Observations) has observed an aerosol enhancement. This enhancement, called the ATAL, has a similar morphology to observed enhancements in long-lived trace gas species like CO. Since the CALIPSO record begins in 2006, the question of how long this aerosol feature has been present requires a new look at the long-lived SAGE II data sets despite significant hurdles to its use in the subtropical upper troposphere. We find that there is no evidence of ATAL in the SAGE II data prior to 1998. After 1998, it is clear that aerosol in the upper troposphere in the ATAL region is substantially enhanced relative to the period before that time. In addition, the data generally supports the presence of the ATAL beginning in 1999 and continuing through the end of the mission, though some years (e.g., 2003) are complicated by the presence of episodic enhancements most likely of volcanic origin.

This study assesses the robustness of the CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) polar stratospheric cloud (PSC) composition classification algorithm – which is based solely on the spaceborne lidar data – through the use of nearly coincident gas-phase HNO3 and H2O data from the Microwave Limb Sounder (MLS) on Aura and Goddard Earth Observing System Model, Version 5 (GEOS-5) temperature analyses. Following the approach of Lambert et al. (2012), we compared the observed temperature-dependent HNO3 uptake by PSCs in the various CALIOP composition classes with modeled uptake for supercooled ternary solutions (STS) and equilibrium nitric acid trihydrate (NAT). We examined the CALIOP PSC data record from both polar regions over the period from 2006 through 2011 and over a range of potential temperature levels spanning the 15–30 km altitude range. We found that most PSCs identified as STS exhibit gas phase uptake of HNO3 consistent with theory, but with a small temperature bias, similar to Lambert et al. (2012). Ice PSC classification is also robust in the CALIOP optical data, with the mode in the ice observations occurring about 0.5 K below the frost point. We found that CALIOP PSCs identified as NAT mixtures exhibit two distinct preferred modes which reflect the fact that the growth of NAT particles is kinetically limited. One mode is significantly out of thermodynamic equilibrium with respect to NAT due to short exposure times to temperatures below the NAT existence temperature, TNAT, with HNO3 uptake dominated by the more numerous liquid droplets. The other NAT mixture mode is much closer to NAT thermodynamic equilibrium, indicating that the particles have been exposed to temperatures below TNAT for extended periods of time. With a few notable exceptions, PSCs in the various composition classes conform well to their expected temperature existence regimes. We have a good understanding of the cause of the minor misclassifications that do occur and will investigate means to correct these deficiencies in our next generation algorithm.

Herein, the Halogen Occultation Experiment (HALOE) aerosol extinction coefficient data is evaluated in the low aerosol loading period after 1996 as the first necessary step in a process that will eventually allow the production of a combined HALOE/SAGE II (Stratospheric Aerosol and Gas Experiment) aerosol climatology of derived aerosol products including surface area density. Based on these analyses, it is demonstrated that HALOE's 3.46 μm is of good quality above 19 km and suitable for scientific applications above that altitude. However, it is increasingly suspect at lower altitudes and should not be used below 17 km under any circumstances after 1996. The 3.40 μm is biased by about 10% throughout the lower stratosphere due to the failure to clear NO2 but otherwise appears to be a high quality product down to 15 km. The 2.45 and 5.26 μm aerosol extinction coefficient measurements are clearly biased and should not be used for scientific applications after the most intense parts of the Pinatubo period. Many of the issues in the aerosol data appear to be related to either the failure to clear some interfering gas species or doing so poorly. For instance, it is clear that the 3.40 μm aerosol extinction coefficient measurements can be improved through the inclusion of an NO2 correction and could, in fact, end up as the highest quality overall HALOE aerosol extinction coefficient measurement. It also appears that the 2.45 and 5.26 μm channels may be improved by updating the Upper Atmosphere Pilot Database which is used as a resource for the removal of gas species otherwise not available from direct HALOE measurements. Finally, a simple model to demonstrate the promise of mixed visible/infrared aerosol extinction coefficient ensembles for the retrieval of bulk aerosol properties demonstrates that a combined HALOE/SAGE II aerosol climatology is feasible and may represent a substantial improvement over independently derived data sets.

SCIAMACHY limb scatter ozone profiles from 2002 to 2008 have been compared with MLS (2005–2008), SABER (2002–2008), SAGE II (2002–2005), HALOE (2002–2005) and ACE-FTS (2004–2008) measurements. The comparison is performed for global zonal averages and heights from 10 to 50 km in one km steps. The validation was performed by comparing monthly mean zonal means and by comparing averages over collocated profiles within a zonal band and month. Both approaches yield similar results. For most of the stratosphere SCIAMACHY agrees to within 10% or better with other correlative data. A systematic bias of SCIAMACHY ozone of up to 100% between 10 and 20 km in the tropics points to some remaining issues with regard to convective cloud interference. Statistical hypothesis testing reveals at which altitudes and in which region differences between SCIAMACHY and other satellite data are statistically significant. We also estimated linear trends from monthly mean data for different periods where SCIAMACHY has common observations with other satellite data using a classical trend model with QBO and seasonal terms in order to draw conclusions on potential instrumental drifts as a function of latitude and altitude. Since the time periods considered here are rather short these trend estimates are only used to identify potential instrumental issues with the SCIAMACHY data. As a result SCIAMACHY exhibits a statistically significant negative trend in the range of of about 1–3% per year depending on latitude during the period 2002–2005 (overlapping with HALOE and SAGE II) and somewhat less during 2002–2008 (overlapping with SABER) in the altitude range of 30–40 km, while in the period 2004–2008 (overlapping with MLS and ACE-FTS) no significant trends are observed. Since all correlative satellite instruments do not show to a very large extent statistically significant trends in any of the time periods considered here, the negative trends observed with SCIAMACHY data point at some remaining instrumental artifact which is most likely related to residual errors in the tangent height registration of SCIAMACHY.

The evolution of aerosols in the tropical upper troposphere/lower stratosphere between June 2006 and October 2009 is examined using the observations of the space borne CALIOP lidar aboard the CALIPSO satellite. Superimposed on several volcanic plumes and soot from an extreme biomass-burning event in 2009, the measurements reveal the existence of fast-cleansing episodes in the lower stratosphere to altitudes as high as 20 km. The cleansing of the layer, which extends from 14 to 20 km, takes place within 1 to 4 months during the southern tropics convective season that transports aerosol-poor tropospheric air into the lower stratosphere. In contrast, the convective season of the Northern Hemisphere summer shows an increase in the particle load at the tropopause consistent with a lofting of air rich with aerosols. These aerosols can consist of surface-derived material such as mineral dust and soot as well as liquid sulfate and organic particles. The flux of tropospheric air during the Southern Hemisphere convective season derived from CALIOP observations is shown to be 5 times at 16 km and 20 times at 19 km larger, respectively, than that associated with flux caused by slow ascent through radiative heating. These results suggest that convective overshooting is a major contributor to troposphere-to-stratosphere transport with concomitant implications for the Tropical Tropopause Layer top height, the humidity, the photochemistry and the thermal structure of the layer.

Spaceborne lidar measurements from CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) are used to provide a vortex-wide perspective of the 2009–2010 Arctic PSC (polar stratospheric cloud) season to complement more focused measurements from the European Union RECONCILE (reconciliation of essential process parameters for an enhanced predictability of Arctic stratospheric ozone loss and its climate interactions) field campaign. The 2009–2010 Arctic winter was unusually cold at stratospheric levels from mid-December 2009 until the end of January 2010, and was one of only a few winters from the past fifty-two years with synoptic-scale regions of temperatures below the frost point. More PSCs were observed by CALIPSO during the 2009–2010 Arctic winter than in the previous three Arctic seasons combined. In particular, there were significantly more observations of high number density NAT (nitric acid trihydrate) mixtures (referred to as Mix 2-enh) and ice PSCs. We found that the 2009–2010 season could roughly be divided into four periods with distinctly different PSC optical characteristics. The early season (15–30 December 2009) was characterized by patchy, tenuous PSCs, primarily low number density liquid/NAT mixtures. No ice clouds were observed by CALIPSO during this early phase, suggesting that these early season NAT clouds were formed through a non-ice nucleation mechanism. The second phase of the season (31 December 2009–14 January 2010) was characterized by frequent mountain wave ice clouds that nucleated widespread NAT particles throughout the vortex, including Mix 2-enh. The third phase of the season (15–21 January 2010) was characterized by synoptic-scale temperatures below the frost point which led to a rare outbreak of widespread ice clouds. The fourth phase of the season (22–28 January) was characterized by a major stratospheric warming that distorted the vortex, displacing the cold pool from the vortex center. This final phase was dominated by STS (supercooled ternary solution) PSCs, although NAT particles may have been present in low number densities, but were masked by the more abundant STS droplets at colder temperatures. We also found distinct variations in the relative proportion of PSCs in each composition class with altitude over the course of the 2009–2010 Arctic season. Lower number density liquid/NAT mixtures were most frequently observed in the lower altitude regions of the clouds (below ~18–20 km), which is consistent with CALIPSO observations in the Antarctic. Higher number density liquid/NAT mixtures, especially Mix 2-enh, were most frequently observed at altitudes above 18–20 km, primarily downstream of wave ice clouds. This pattern is consistent with the conceptual model whereby low number density, large NAT particles are precipitated from higher number density NAT clouds (i.e. mother clouds) that are nucleated downstream of mountain wave ice clouds.

Herein, we provide an assessment of the data quality of Stratospheric Aerosol and Gas Experiment (SAGE III) Version 4 aerosol extinction coefficient and water vapor data products. The evaluation is based on comparisons with data from four instruments: SAGE II, the Polar Ozone and Aerosol Measurement (POAM III), the Halogen Occultation Experiment (HALOE), and the Microwave Limb Sounder (MLS). Since only about half of the SAGE III channels have a direct comparison with measurements by other instruments, we have employed some empirical techniques to evaluate measurements at some wavelengths. We find that the aerosol extinction coefficient measurements at 449, 520, 755, 869, and 1021 nm are reliable with accuracies and precisions on the order of 10% in the mission's primary aerosol target range of 15 to 25 km. We also believe this to be true of the aerosol measurements at 1545 nm though we cannot exclude some positive bias below 15 km. We recommend use of the 385 nm measurements above 16 km where the accuracy is on par with other aerosol channels. The 601 nm measurement is much noisier (~20%) than other channels and we suggest caution in the use of these data. We believe that the 676 nm data are clearly defective particularly above 20 km (accuracy as poor as 50%) and the precision is also low (~30%). We suggest excluding this channel under most circumstances. The SAGE III Version 4 water vapor data product appears to be high quality and is recommended for science applications in the stratosphere below 45 km. In this altitude range, the mean differences with all four corroborative data sets are no bigger than 15% and often less than 10% with exceptional agreement with POAM III and MLS. Above 45 km, it seems likely that SAGE III water vapor values are increasingly too large and should be used cautiously or avoided. We believe that SAGE III meets its preflight goal of 15% accuracy and 10% precision between 15 and 45 km. SAGE III water vapor data does not appear to be affected by aerosol loading in the stratosphere.

Solar occultation has proven to be a reliable technique for the measurement of atmospheric constituents in the stratosphere. NASA's Stratospheric Aerosol and Gas Experiments (SAGE, SAGE II, and SAGE III) together have provided over 25 years of quality solar occultation data, a data record which has been an important resource for the scientific exploration of atmospheric composition and climate change. Herein, we describe an improvement to the processing of SAGE data that corrects for a previously uncorrected short-term time-dependence in the calibration function. The variability relates to the apparent rotation of the scanning track with respect to the face of the sun due to the motion of the satellite. Correcting for this effect results in a decrease in the measurement noise in the Level 1 line-of-sight optical depth measurements of approximately 40% in the middle and upper stratospheric SAGE II and III observations where it has been applied. The technique is potentially useful for any scanning solar occultation instrument and suggests further improvement for future occultation measurements if a full disk imaging system can be included.

This paper focuses on polar stratospheric cloud (PSC) measurements by the CALIOP (Cloud-Aerosol LIdar with Orthogonal Polarization) lidar system onboard the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) spacecraft, which has been operating since June 2006. We describe a second-generation PSC detection algorithm that utilizes both the CALIOP 532-nm scattering ratio (ratio of total-to-molecular backscatter coefficients) and 532-nm perpendicular backscatter coefficient measurements for cloud detection. The inclusion of the perpendicular backscatter measurements enhances the detection of tenuous PSC mixtures containing low number densities of solid (likely nitric acid trihydrate, NAT) particles and leads to about a 15% increase in PSC areal coverage compared with our original algorithm. Although these low number density NAT mixtures would have a minimal impact on chlorine activation due to their relatively small particle surface area, these particles may play a significant role in denitrification and therefore are an important component of our PSC detection. In addition, the new algorithm allows discrimination of PSCs by composition in terms of their ensemble backscatter and depolarization in a manner analogous to that used in previous ground-based and airborne lidar PSC studies. Based on theoretical optical calculations, we define four CALIPSO-based composition classes which we call supercooled ternary solution (STS), ice, and Mix1 and Mix2, denoting mixtures of STS with NAT particles in lower or higher number densities/volumes, respectively. We examine the evolution of PSCs for three Antarctic and two Arctic seasons and illustrate the unique attributes of the CALIPSO PSC database. These analyses show substantial interannual variability in PSC areal coverage and also the well-known contrast between the Antarctic and Arctic. The CALIPSO data also reveal seasonal and altitudinal variations in Antarctic PSC composition, which are related to changes in HNO3 and H2O observed by the Microwave Limb Sounder on the Aura satellite.

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.

Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, during background periods, the SAD operational product has an uncertainty of at least a factor of 2 due to the lack of sensitivity to particles with radii less than 100 nm.

The role of polar stratospheric clouds in polar ozone loss has been well documented. The CALIPSO satellite mission offers a new opportunity to characterize PSCs on spatial and temporal scales previously impossible. A PSC detection algorithm based on a single wavelength threshold approach has been developed for CALIPSO. The method appears to accurately detect PSCs of all opacities, including tenuous clouds, with a very low rate of false positives and few missed clouds. We applied the algorithm to CALIOP data acquired during the 2006 Antarctic winter season from 13 June through 31 October. The spatial and temporal distribution of CALIPSO PSC observations is illustrated with weekly maps of PSC occurrence. The evolution of the 2006 PSC season is depicted by time series of daily PSC frequency as a function of altitude. Comparisons with "virtual" solar occultation data indicate that CALIPSO provides a different view of the PSC season than attained with previous solar occultation satellites. Measurement-based time series of PSC areal coverage and vertically-integrated PSC volume are computed from the CALIOP data. The observed area covered with PSCs is significantly smaller than would be inferred from the commonly used temperature-based proxy TNAT but is similar in magnitude to that inferred from TSTS. The potential of CALIOP measurements for investigating PSC composition is illustrated using combinations of lidar backscatter and volume depolarization for two CALIPSO PSC scenes.

We have examined the 532-nm aerosol backscatter coefficient measurements by the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) for their use in the monitoring of stratospheric aerosol. CALIPSO makes observations that span from 82° S to 82° N each day and, for each profile, backscatter coefficient values reported up to ~40 km. The possibility of using CALIPSO for stratospheric aerosol monitoring is demonstrated by the clear observation of the 20 May 2006 eruption of Montserrat in the earliest CALIPSO data in early June as well as by observations showing the 7 October 2006 eruption of Tavurvur (Rabaul). However, the very low aerosol loading within the stratosphere makes routine observations of the stratospheric aerosol far more difficult than relatively dense volcanic plumes. Nonetheless, we found that averaging a complete days worth of nighttime-only data into 5-deg latitude by 1-km vertical bins yields a stratospheric aerosol distribution that is fairly consistent with past measurements by spaceborne instruments. Based on comparisons with 2004 data from the Stratospheric Aerosol and Gas Experiment, the derived values are close to expectation except in the tropics where they are larger by about a factor of 2. The cause of the difference in the tropics is not readily apparent but is most likely related to difficulties in the lidar calibration process currently found in the CALIOP data at tropical latitudes.

The use of SAGE III multiwavelength aerosol extinction coefficient measurements to infer PSC type is contingent on the robustness of both the extinction magnitude and its spectral variation. Past validation with SAGE II and other similar measurements has shown that the SAGE III extinction coefficient measurements are reliable though the comparisons have been greatly weighted toward measurements made at mid-latitudes. Some aerosol comparisons made in the Arctic winter as a part of SOLVE II suggested that SAGE III values, particularly at longer wavelengths, are too small with the implication that both the magnitude and the wavelength dependence are not reliable. Comparisons with POAM III have also suggested a similar discrepancy. Herein, we use SAGE II data as a common standard for comparison of SAGE III and POAM III measurements in the Arctic winters of 2002/2003 through 2004/2005. During the winter, SAGE II measurements are made infrequently at the same latitudes as these instruments. We have mitigated this problem through the use of potential vorticity as a spatial coordinate and thus greatly increased of the number of coincident events. We find that SAGE II and III extinction coefficient measurements show a high degree of compatibility at both 1020 nm and 450 nm except a 10–20% bias at both wavelengths. In addition, the 452 to 1020 nm extinction ratio shows a consistent bias of ~30% throughout the lower stratosphere. We also find that SAGE II and POAM III are on average consistent though the comparisons show a much higher variability and larger bias than SAGE II/III comparisons. In addition, we find that SAGE II and POAM III data sets are not well correlated at and below 18 km. Overall, we find both the extinction values and the spectral dependence from SAGE III are robust and we find no evidence of a significant defect within the Arctic vortex.

The Gas and Aerosol Measurement Sensor (GAMS) was deployed aboard the NASA DC-8 aircraft during the second SAGE III Ozone Loss and Validation Experiment (SOLVE II). GAMS acquired line-of-sight (LOS) direct solar irradiance spectra during the sunlit portions of ten science flights of the DC-8 between 12 January and 4 February 2003. Differential line-of-sight (DLOS) optical depth spectra are produced from the GAMS raw solar irradiance spectra. Then, DLOS ozone number densities are retrieved from the GAMS spectra using a multiple linear regression spectral fitting technique. Both the DLOS optical depth spectra and retrieved ozone data are compared with coincident measurements from two other solar instruments aboard the DC-8 platform to demonstrate the robustness and stability of the GAMS data. The GAMS ozone measurements are then utilized to evaluate the quality of the Wulf band ozone cross sections, a critical component of the SAGE III aerosol, water vapor, and temperature/pressure retrievals. Results suggest the ozone cross section compilation of Shettle and Anderson currently used operationally in SAGE III data processing may be in error by as much as 10–20% in the Wulf bands, and their lack of reported temperature dependence is a significant deficiency. A second, more recent, cross section database compiled for the SCIAMACHY satellite mission appears to be of much better quality in the Wulf bands, but still may have errors as large as 5% near the Wulf band absorption peaks, which is slightly larger than their stated uncertainty. Additional laboratory measurements of the Wulf band cross sections should be pursued to further reduce their uncertainty and better quantify their temperature dependence.

During the 2003 SAGE (Stratospheric Aerosol and Gas Experiment) III Ozone Loss and Validation Experiment (SOLVE) II, the fourteen-channel NASA Ames Airborne Tracking Sunphotometer (AATS-14) was mounted on the NASA DC-8 aircraft and measured spectra of total and aerosol optical depth (TOD and AOD) during the sunlit portions of eight science flights. Values of ozone column content above the aircraft have been derived from the AATS-14 measurements by using a linear least squares method that exploits the differential ozone absorption in the seven AATS-14 channels located within the Chappuis band. We compare AATS-14 columnar ozone retrievals with temporally and spatially near-coincident measurements acquired by the SAGE III and the Polar Ozone and Aerosol Measurement (POAM) III satellite sensors during four solar occultation events observed by each satellite. RMS differences are 19 DU (7% of the AATS value) for AATS-SAGE and 10 DU (3% of the AATS value) for AATS-POAM. In these checks of consistency between AATS-14 and SAGE III or POAM III ozone results, the AATS-14 analyses use airmass factors derived from the relative vertical profiles of ozone and aerosol extinction obtained by SAGE III or POAM III. We also compare AATS-14 ozone retrievals for measurements obtained during three DC-8 flights that included extended horizontal transects with total column ozone data acquired by the Total Ozone Mapping Spectrometer (TOMS) and the Global Ozone Monitoring Experiment (GOME) satellite sensors. To enable these comparisons, the amount of ozone in the column below the aircraft is estimated either by assuming a climatological model or by combining SAGE and/or POAM data with high resolution in-situ ozone measurements acquired by the NASA Langley Research Center chemiluminescent ozone sensor, FASTOZ, during the aircraft vertical profile at the start or end of each flight. Resultant total column ozone values agree with corresponding TOMS and GOME measurements to within 10-15 DU (~3%) for AATS data acquired during two flights - a longitudinal transect from Sweden to Greenland on 21 January, and a latitudinal transect from 47° N to 35° N on 6 February. For the round trip DC-8 latitudinal transect between 34° N and 22° N on 19-20 December 2002, resultant AATS-14 ozone retrievals plus below-aircraft ozone estimates yield a latitudinal gradient that is similar in shape to that observed by TOMS and GOME, but resultant AATS values exceed the corresponding satellite values by up to 30 DU at certain latitudes. These differences are unexplained, but they are attributed to spatial and temporal variability that was associated with the dynamics near the subtropical jet but was unresolved by the satellite sensors. For selected cases, we also compare AATS-14 ozone retrievals with values derived from coincident measurements by the other two DC-8 based solar occultation instruments: the National Center for Atmospheric Research Direct beam Irradiance Airborne Spectrometer (DIAS) and the NASA Langley Research Center Gas and Aerosol Monitoring System (GAMS). AATS and DIAS retrievals agree to within RMS differences of 1% of the AATS values for the 21 January and 19-20 December flights, and 2.3% for the 6 February flight. Corresponding AATS-GAMS RMS differences are ~1.5% for the 21 January flight; GAMS data were not compared for the 6 February flight and were not available for the 19-20 December flight. Line of sight ozone retrievals from coincident measurements obtained by the three DC-8 solar occultation instruments during the SAGE III solar occultation event on 24 January yield RMS differences of 2.1% for AATS-DIAS and 0.5% for AATS-GAMS.