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Vertical ozone profiles from combined spectral measurements in the ultraviolet and infrared spectral range were retrieved by using data from the TROPOspheric Monitoring Instrument on the Sentinel-5 Precursor (TROPOMI/S5P) and the Cross-track Infrared Sounder on the Suomi National Polar-orbiting Partnership (CrIS/Suomi-NPP), which are flying in loose formation 3 min apart in the same orbit. A previous study of ozone profiles retrieved exclusively from TROPOMI UV spectra showed that the vertical resolution in the troposphere is clearly limited (Mettig et al., 2021). The vertical resolution and the vertical extent of the ozone profiles is improved by combining both wavelength ranges compared to retrievals limited to UV or IR spectral data only. The combined retrieval particularly improves the accuracy of the retrieved tropospheric ozone and to a lesser degree stratospheric ozone up to 30 km. An increase in the degrees of freedom (DOF) by 1 DOF was found in the UV + IR retrieval compared to the UV-only retrieval. Compared to previous publications, which investigated combinations of UV and IR observations from the Ozone Monitoring Instrument and Tropospheric Emission Spectrometer (OMI and TES) and Global Ozone Monitoring Experiment version 2 and Infrared Atmospheric Sounding Interferometer (GOME-2 and IASI) pairs, the degree of freedom is lower, which is attributed to the reduced spectral resolution of CrIS compared to TES or IASI. Tropospheric lidar and ozonesondes were used to validate the ozone profiles and tropospheric ozone content (TOC). In their comparison with tropospheric lidars, both ozone profiles and TOCs show smaller biases for the retrieved data from the combined UV + IR observation than from the UV observations alone. For the ozone profiles below 10 km, the mean differences are around ±10 % and the mean TOC varies around ±3 DU. We show that TOCs from the combined retrieval agree better with ozonesonde results at northern latitudes than the UV-only and IR-only retrievals and also have lower scatter. In the tropics, the IR-only retrieval shows the best agrement with TOCs derived from ozonesondes. While in general the TOCs show good agreement with ozonesonde data, the profiles have a positive bias of around 30 % between 10 and 15 km. The reason is probably a positive stratospheric bias from the IR retrieval. The comparison of the UV + IR and UV ozone profiles up to 30 km with the Microwave Limb Sounder (MLS) demonstrates the improvement of the UV + IR profile in the stratosphere above 18 km. In comparison to the UV-only approach the retrieval shows improvements of up to 10 % depending on latitude but can also show worse results in some regions and latitudes.

The Geostationary Environment Monitoring Spectrometer (GEMS) is scheduled for launch in February 2020 to monitor air quality (AQ) at an unprecedented spatial and temporal resolution from a geostationary Earth orbit (GEO) for the first time. With the development of UV–visible spectrometers at sub-nm spectral resolution and sophisticated retrieval algorithms, estimates of the column amounts of atmospheric pollutants (O3, NO2, SO2, HCHO, CHOCHO, and aerosols) can be obtained. To date, all the UV–visible satellite missions monitoring air quality have been in low Earth orbit (LEO), allowing one to two observations per day. With UV–visible instruments on GEO platforms, the diurnal variations of these pollutants can now be determined. Details of the GEMS mission are presented, including instrumentation, scientific algorithms, predicted performance, and applications for air quality forecasts through data assimilation. GEMS will be on board the Geostationary Korea Multi-Purpose Satellite 2 (GEO-KOMPSAT-2) satellite series, which also hosts the Advanced Meteorological Imager (AMI) and Geostationary Ocean Color Imager 2 (GOCI-2). These three instruments will provide synergistic science products to better understand air quality, meteorology, the long-range transport of air pollutants, emission source distributions, and chemical processes. Faster sampling rates at higher spatial resolution will increase the probability of finding cloud-free pixels, leading to more observations of aerosols and trace gases than is possible from LEO. GEMS will be joined by NASA’s Tropospheric Emissions: Monitoring of Pollution (TEMPO) and ESA’s Sentinel-4 to form a GEO AQ satellite constellation in early 2020s, coordinated by the Committee on Earth Observation Satellites (CEOS).

The NASA Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) project included goals related to aerosol particle life cycle in convective regimes. Using the University of Wisconsin High Spectral Resolution Lidar system at Huntsville, Alabama, USA, and the NASA DC-8 research aircraft, we investigate the altitude dependence of aerosol, water vapor and Altocumulus (Ac) properties in the free troposphere from a canonical 12 August 2013 convective storm case as a segue to a presentation of a mission-wide analysis. It stands to reason that any moisture detrainment from convection must have an associated aerosol layer. Modes of covariability between aerosol, water vapor and Ac are examined relative to the boundary layer entrainment zone, 0 ∘C level, and anvil, a region known to contain Ac clouds and a complex aerosol layering structure (Reid et al., 2017). Multiple aerosol layers in regions warmer than 0 ∘C were observed within the planetary boundary layer entrainment zone. At 0 ∘C there is a proclivity for aerosol and water vapor detrainment from storms, in association with melting level Ac shelves. Finally, at temperatures colder than 0 ∘C, weak aerosol layers were identified above Cumulus congestus tops (∼0 and ∼-20 ∘C). Stronger aerosol signals return in association with anvil outflow. In situ data suggest that detraining particles undergo aqueous-phase or heterogeneous chemical or microphysical transformations, while at the same time larger particles are being scavenged at higher altitudes leading to enhanced nucleation. We conclude by discussing hypotheses regarding links to aerosol emissions and potential indirect effects on Ac clouds.

The conventional two-wavelength differential absorption lidar (DIAL) has measured air pollutants such as nitrogen dioxide (NO2). However, high concentrations of aerosol within the planetary boundary layer (PBL) can cause significant retrieval errors using only a two-wavelength DIAL technique to measure NO2. We proposed a new technique to obtain more accurate measurements of NO2 using a three-wavelength DIAL technique based on an optical parametric oscillator (OPO) laser. This study derives the three-wavelength DIAL retrieval equations necessary to retrieve vertical profiles of NO2 in the troposphere. Additionally, two rules to obtain the optimum choice of the three wavelengths applied in the retrieval are designed to help increase the differences in the NO2 absorption cross-sections and reduce aerosol interference. NO2 retrieval relative uncertainties caused by aerosol extinction, molecular extinction, absorption of gases other than the gas of interest and backscattering are calculated using two-wavelength DIAL (438 and 439.5 nm) and three-wavelength DIAL (438, 439.5 and 441 nm) techniques. The retrieval uncertainties in aerosol extinction using the three-wavelength DIAL technique are reduced to less than 2 % of those when using the two-wavelength DIAL technique. Moreover, the retrieval uncertainty analysis indicates that the three-wavelength DIAL technique can reduce more fluctuation caused by aerosol backscattering than the two-wavelength DIAL technique. This study presents NO2 concentration profiles which were obtained using the HU (Hampton University) three-wavelength OPO DIAL. As a first step to assess the accuracy of the HU lidar NO2 profiles, we compared the NO2 profiles to simulated data from the Weather Research and Forecasting Chemistry (WRF-Chem) model. This comparison suggests that the NO2 profiles retrieved with the three-wavelength DIAL technique have similar vertical structure and magnitudes typically within ±0.1 ppb compared to modeled profiles.

TEMPO was selected in 2012 by NASA as the first Earth Venture Instrument, for launch between 2018 and 2021. It will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO observes from Mexico City, Cuba, and the Bahamas to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution (~2.1 km N/S×4.4 km E/W at 36.5°N, 100°W). TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry, as well as contributing to carbon cycle knowledge. Measurements are made hourly from geostationary (GEO) orbit, to capture the high variability present in the diurnal cycle of emissions and chemistry that are unobservable from current low-Earth orbit (LEO) satellites that measure once per day. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a commercial GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve ozone (O), nitrogen dioxide (NO), sulfur dioxide (SO), formaldehyde (HCO), glyoxal (CHO), bromine monoxide (BrO), IO (iodine monoxide), water vapor, aerosols, cloud parameters, ultraviolet radiation, and foliage properties. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O chemistry cycle. Multi-spectral observations provide sensitivity to O in the lowermost troposphere, substantially reducing uncertainty in air quality predictions. TEMPO quantifies and tracks the evolution of aerosol loading. It provides these near-real-time air quality products that will be made publicly available. TEMPO will launch at a prime time to be the North American component of the global geostationary constellation of pollution monitoring together with the European Sentinel-4 (S4) and Korean Geostationary Environment Monitoring Spectrometer (GEMS) instruments.

Aerosol retrieval using ozone lidars in the ultraviolet (UV) band is challenging but necessary for correcting aerosol interference in ozone retrieval and for studying the ozone-aerosol correlations. This study describes the aerosol retrieval algorithm for a tropospheric ozone lidar, quantifies the retrieval error budget, and intercompares the aerosol retrieval products at 299 nm with those at 532 nm from a high spectral resolution lidar (HSRL). After the cloud-contaminated data is filtered out, the aerosol backscatter or extinction coefficients at a 30-m and 10-min resolution retrieved by the ozone lidar are highly correlated with the HSRL products, with a coefficient of 0.95 suggesting that the ozone lidar can reliably measure aerosol structures with high spatio-temporal resolution when the signal-to-noise ratio is sufficient. The actual uncertainties of the aerosol retrieval from the ozone lidar generally agree with our theoretical analysis. The backscatter color ratio (backscatter-related exponent of wavelength dependence) linking the coincident data measured by the two instruments at 299 and 532 nm is 1.34 ± 0.11 while the Ångström (extinction-related) exponent is 1.49 ± 0.16 for a mixture of urban and fire smoke aerosols within the troposphere above Huntsville, AL, USA.

As part of the Southeast United States based Studies of Emissions & Atmospheric Composition, Clouds & Climate Coupling by Regional Surveys (SEAC4RS), and collinear with part of the Southeast Atmosphere Study (SAS), the University of Wisconsin High Spectral Resolution Lidar (UW-HSRL) system was deployed to the University of Alabama from June 19th through November 4th, 2013. With a collocated Aerosol Robotic NETwork (AERONET) sun photometer, a nearby Chemical Speciation Network (PM2.5) measurement station, and near daily ozonesonde releases for the August-September SEAC4RS campaign, the site allowed the region's first comprehensive diurnal monitoring of aerosol particle vertical structure. A 532 nm lidar ratio of 55 sr provided good closure between aerosol backscatter and AERONET Aerosol Optical Thickness (AOT). A principle component analysis was performed to identify key modes of variability in aerosol backscatter. “Fair weather” days exhibited classic planetary boundary layer (PBL) structure of a mixed layer accounting for ~50% of AOT and an entrainment zone providing another 25%. An additional 5-15% of variance is gained from the lower free troposphere from either convective detrainment or frequent intrusions of Western United States biomass burning smoke. Generally aerosol particles were contained below the 0o C level, a common level of stability in convective regimes. However, occasional strong injections of smoke to the upper troposphere were also observed, accounting for the remaining 10-15% variability in AOT. Examples of these common modes of variability in frontal and convective regimes are presented, demonstrating why AOT often has only a weak relationship to surface PM2.5 concentration.

Stratosphere-to-troposphere transport (STT) and biomass burning (BB) are two important natural sources for tropospheric ozone that can result in elevated ozone and air-quality episode events. High-resolution observations of multiple related species are critical for complex ozone source attribution. In this article, we present an analysis of coinciding ground-based and airborne observations, including ozone lidar, ozonesonde, high spectral resolution lidar (HSRL), and multiple airborne in situ measurements, made on 28 and 29 June 2013 during the Southeast Nexus field campaign. The ozone lidar and HSRL reveal detailed ozone and aerosol structures as well as the temporal evolution associated with a cold front passage. The observations also captured two enhanced (+30 ppbv) ozone layers in the free troposphere (FT), which were determined from this study to be caused by a mixture of BB and stratospheric sources. The mechanism for this STT is tropopause folding associated with a cutoff upper level low-pressure system according to the analysis of its potential vorticity structure. The depth of the tropopause fold appears to be shallow for this case compared to events observed in other seasons; however, the impact on lower tropospheric ozone was clearly observed. This event suggests that strong STT may occur in the southeast United States during the summer and can potentially impact lower troposphere during these times. Statistical analysis of the airborne observations of trace gases suggests a coincident influence of BB transport in the FT impacting the vertical structure of ozone during this case study.

The NASA/Smithsonian Tropospheric Emissions: Monitoring of Pollution (TEMPO; tempo.si.edu) satellite instrument will measure atmospheric pollution and much more over Greater North America at high temporal resolution (hourly or better in daylight, with selected observations at 10 minute or better sampling) and high spatial resolution (10 km2 at the center of the field of regard). It will measure ozone (O3) profiles (including boundary layer O3), and columns of nitrogen dioxide (NO2), nitrous acid (HNO2), sulfur dioxide (SO2), formaldehyde (H2CO), glyoxal (C2H2O2), water vapor (H2O), bromine oxide (BrO), iodine oxide (IO), chlorine dioxide (OClO), as well as clouds and aerosols, foliage properties, and ultraviolet B (UVB) radiation. The instrument has been delivered and is awaiting spacecraft integration and launch in 2022. This talk describes a selection of TEMPO applications based on the TEMPO Green Paper living document (http://tempo.si.edu/publications.html). Applications to air quality and health will be summarized. Other applications presented include: biomass burning and O3 production; aerosol products including synergy with GOES infrared measurements; lightning NOx; soil NOx and fertilizer application; crop and forest damage from O3; chlorophyll and primary productivity; foliage studies; halogens in coastal and lake regions; ship tracks and drilling platform plumes; water vapor studies including atmospheric rivers, hurricanes, and corn sweat; volcanic emissions; air pollution and economic evolution; high-resolution pollution versus traffic patterns; tidal effects on estuarine circulation and outflow plumes; air quality response to power blackouts and other exceptional events.

We investigated the diurnal ozone variation on 6 September 2013 in a midsize urban environment using multiple in situ and remote-sensing measurements along with the Dutch atmospheric large-eddy simulation (DALES) model coupled with a chemical module and a dry deposition module that we added for this study. Our study area was Huntsville, Alabama, USA, a typical midsize city in the Southeastern United States. The ozone variation in the convective boundary layer (CBL) resulted mainly from local emissions and photochemical production stemming from weather conditions controlled by an anticyclonic system on that day. Local chemical production contributes approximately two thirds of the ozone enhancement in the CBL and, in this case, dynamical processes including ozone transport from the free troposphere (FT) to the CBL through the entrainment processes contributed the remainder. The numerical experiments performed by the large-eddy simulation (LES) model showed acceptable agreement with the TOLNet (The tropospheric ozone lidar network)/RO3QET (Rocket-city ozone quality evaluation in the troposphere) ozone DIAL (differential absorption lidar) observations. This study indicated the need for fine-scale, three-dimensional ozone observations with high temporal and spatial resolution for air quality studies at the urban scale and smaller.

The NASA Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) project included goals related to aerosol particle life cycle in convective regimes. Using the University of Wisconsin High Spectral Resolution Lidar system at Huntsville, Alabama, USA, and the NASA DC-8 research aircraft, we investigate the altitude dependence of aerosol, water vapor and Altocumulus (Ac) properties in the free troposphere from a canonical 12 August 2013 convective storm case as a segue to a presentation of a mission-wide analysis. It stands to reason that any moisture detrainment from convection must have an associated aerosol layer. Modes of covariability between aerosol, water vapor and Ac are examined relative to the boundary layer entrainment zone, 0 ∘C level, and anvil, a region known to contain Ac clouds and a complex aerosol layering structure (Reid et al., 2017). Multiple aerosol layers in regions warmer than 0 ∘C were observed within the planetary boundary layer entrainment zone. At 0 ∘C there is a proclivity for aerosol and water vapor detrainment from storms, in association with melting level Ac shelves. Finally, at temperatures colder than 0 ∘C, weak aerosol layers were identified above Cumulus congestus tops (∼0 and ∼-20 ∘C). Stronger aerosol signals return in association with anvil outflow. In situ data suggest that detraining particles undergo aqueous-phase or heterogeneous chemical or microphysical transformations, while at the same time larger particles are being scavenged at higher altitudes leading to enhanced nucleation. We conclude by discussing hypotheses regarding links to aerosol emissions and potential indirect effects on Ac clouds.

In troposphere, ozone is a toxic secondary pollutant produced when its precursors react in sunlight. An important source of ozone precursors is biomass burning. Here we investigate the impacts of 2016 Southeast U.S. Wildfires on ozone production by integrating vertical resolved ozone profiles and photochemical modeling. The results show that wildfires contributed to ozone lamina at the top of boundary layer and enhanced surface ozone up to about 10ppbv in Southeast U.S.. Ozone lidar observed a lower ozone change with respect to a fast growth of aerosol plume, of which the reason is also investigated. Current results indicate an effective integration of vertical observations and modeling for us to understand the ozone production from fires in troposphere.

The North-America-based Tropospheric Ozone Lidar Network (TOLNet) was recently established to provide high spatio-temporal vertical profiles of ozone, to better understand physical processes driving tropospheric ozone variability, and to validate the tropospheric ozone measurements of upcoming space-borne missions such as Tropospheric Emissions: Monitoring Pollution (TEMPO). The network currently comprises six tropospheric ozone lidars, four of which are mobile instruments deploying to the field a few times per year, based on campaign and science needs. In August 2016, all four mobile TOLNet lidars were brought to the fixed TOLNet site of JPL-Table Mountain Facility for the one-week-long Southern California Ozone Observation Project (SCOOP). This inter-comparison campaign, which included 400 hours of lidar measurements and 18 ozonesondes launches, allowed for the unprecedented simultaneous validation of five of the six TOLNet lidars. For measurements between 3 and 10 km above sea level, a mean difference of 0.7 ppbv (1.7 %), with a root-mean-square deviation of 1.6 ppbv or 2.4 % was found between the lidars and ozonesondes, which is well within the combined uncertainties of the two measurement techniques. The few minor differences identified were typically associated with the known limitations of the lidars at the profiles altitude extremes (i.e., first 1 km above ground and at the instruments highest retrievable altitude). As part of a large homogenization and quality control effort within the network, many aspects of the TOLNet in-house data processing algorithms were also standardized and validated. This thorough validation of both the measurements and retrievals builds confidence in the high quality and reliability of the TOLNet ozone lidar profiles for many years to come, making TOLNet a valuable ground-based reference network for tropospheric ozone profiling.

Potential sources of a priori ozone (O3) profiles for use in Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite tropospheric O3 retrievals are evaluated with observations from multiple Tropospheric Ozone Lidar Network (TOLNet) systems in North America. An O3 profile climatology (tropopause-based O3 climatology (TB-Clim), currently proposed for use in TEMPO O3 retrieval algorithms) based on ozonesonde observations and O3 profiles from 3 separate models (operational Goddard Earth Observing System (GEOS-5) Forward Processing (FP) product, reanalysis product from Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA2), and the GEOS-Chem chemical transport model (CTM)) were: 1) evaluated with TOLNet measurements on various temporal scales (seasonally, daily, hourly) and 2) implemented as a priori information in theoretical TEMPO tropospheric O3 retrievals in order to determine how each a priori impacts the accuracy of retrieved tropospheric (0–10 km) and lowermost tropospheric (LMT, 0–2 km) O3 columns. We found that all potential sources of a priori profiles evaluated in this study generally reproduced the vertical structure of summer-averaged observations of O3 profiles. However, larger differences between the a priori profiles and lidar observations were observed when evaluating inter-daily and diurnal variability of tropospheric O3. The TB-Clim O3 profile climatology was unable to replicate observed inter-daily and diurnal variability of O3 while model products, in particular GEOS-Chem simulations, displayed more skill in reproducing these features. Due to the ability of models, primarily the CTM used in this study, on average to capture the inter-daily and diurnal variability of tropospheric and LMT O3 columns, using a priori profiles from these model simulations resulted in TEMPO retrievals with the best statistical comparison with lidar observations. Furthermore, important from an air quality perspective, when high LMT O3 values are observed, using GEOS-Chem a priori profiles resulted in TEMPO LMT O3 retrievals with the least bias.

International audience; Ground-based lidars and ozonesondes belonging to the NASA-supported Tropospheric Ozone Lidar Network (TOLNet) are used in conjunction with the NASA Alpha Jet Atmospheric eXperiment (AJAX) to investigate the transport of stratospheric ozone and entrained pollution into the lower troposphere above the United States on May 24–25, 2013. TOLNet and AJAX measurements made in California, Nevada, and Alabama are compared to tropospheric ozone retrievals from the Atmospheric Infrared Sounder (AIRS), to back trajectories from the NOAA Air Resources Laboratory (ARL) Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model, and to analyses from the NOAA/NESDIS Real-time Air Quality Modeling System (RAQMS) and FLEXPART particle dispersion model. The measurements and model analyses show much deeper descent of ozone-rich upper tropospheric/lower stratospheric air above the Desert Southwest than above the Southeast, and comparisons to surface measurements from regulatory monitors reporting to the U.S. EPA Air Quality System (AQS) suggest that there was a much greater surface impact in the Southwest including exceedances of the 2008 National Ambient Air Quality Standard (NAAQS) of 0.075 ppm in both Southern California and Nevada. Our analysis demonstrates the potential benefits to be gained by supplementing the existing surface ozone network with coordinated upper air observations by TOLNet.

Recently, we successfully demonstrated a new compact and robust ozone DIAL lidar for smaller aircraft such as the NASA B200 and the ER-2 high-altitude aircraft. This is the first NASA airborne lidar to incorporate advanced solid-state lasers to produce the required power at the required ultraviolet wavelengths, and is compact and robust enough to operate nearly autonomously on the high-altitude ER-2 aircraft. This technology development resulted in the first new NASA airborne ozone DIAL instrument in more than 15 years. The combined ozone, aerosol, and clouds measurements provide valuable information on the chemistry, radiation, and dynamics of the atmosphere. In particular, from the ER-2 it offers a unique capability to study the upper troposphere and lower stratosphere.

Five TOLNet lidars participated to a validation campaign at the JPL-Table Mountain Facility, CA in August 2016. All lidars agreed within ±10% of each other and within ±7% of the ozonesondes. Centralized data processing was used to compare the uncertainty budgets. The results highlight the TOLNet potential to address science questions ranging from boundary layer processes to long range transport. TOLNet can now be seen as a robust network for use in field campaigns and long term monitoring.

The Tropospheric Ozone Lidar Network (TOLNet) is a unique network of lidar systems that measure atmospheric profiles of ozone and aerosols, to contribute to air-quality studies, atmospheric modeling, and satellite validation efforts. The accurate characterization of these lidars is of critical interest, and is necessary to determine cross-instrument calibration uniformity. From July to August 2014, three lidars, the TROPospheric OZone (TROPOZ) lidar, the Tunable Optical Profiler for Aerosol and oZone (TOPAZ) lidar, and the Langley Mobile Ozone Lidar (LMOL), of TOLNet participated in the “Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality” (DISCOVER-AQ) mission and the “Front Range Air Pollution and Photochemistry Éxperiment” (FRAPPÉ) to measure sub-hourly ozone variations from near the surface to the top of the troposphere. Although large differences occur at few individual altitudes in the near field and far field range, the TOLNet lidars agree with each other within ±4%. These results indicate excellent measurement accuracy for the TOLNet lidars that is suitable for use in air-quality and ozone modeling efforts.

High spatial- and temporal-resolution ozone lidar profiles, in conjunction with ozonesonde and satellite observations, are well suited to characterize short-term ozone variations due to different physical and chemical processes, such as the impact of lightning-generated NOx (LNOx) on tropospheric ozone. This work presents the hourly variation of tropospheric-ozone profiles measured by an ozone lidar at the University of Alabama in Huntsville, on July 14, 18, and 27, 2011. These ozone lidar data are compared with two WRF/Chem simulations, one with lightning NO (LNO) emissions and the other without. On July 14, 2011, the ozone lidar observed an ozone laminar structure with elevated ozone concentrations of 65∼80 ppbv below 2 km, low ozone (50∼65) ppbv between 2 and 5 km, and high ozone up to 165 ppbv between 5 and 12 km AGL. WRF/Chem simulations, in conjunction with backward trajectory analysis, suggest that lightning events occurring within upwind regions resulted in an ozone enhancement of 28 ppbv at 7.5 km AGL over Huntsville. On July 27, LNO emissions were transported to Huntsville from upwind and account for 75% of NOx and an 8.3 ppbv of ozone enhancement at ∼10 km; the model overestimates ozone between 2.5 and 5 km AGL.

Ozone laminae result from complex chemical and dynamical processes in the atmosphere. Unfortunately, there is no accepted definition of ozone laminae due to limited knowledge of the science determining their formation and evolution. Current methods to define ozone laminae are based on a reference profile that results from smoothing or linearly-regressing the original profile. These definitions are likely to underestimate the number of ozone laminae in the troposphere because the production of reference profiles reduces the information content in the original profiles. We present a method using the Continuous Wavelet Transform (CWT) with a two-threshold technique to define ozone laminae number and magnitude without requiring a reference profile. Our method encompasses an efficient and robust capability for identifying ozone laminae in the 15-year ozone profiles observed by ozonesondes in Huntsville, AL.

Tropospheric ozone variability occurs because of multiple forcing factors including surface emission of ozone precursors, stratosphere-to-troposphere transport (STT), and meteorological conditions. Analyses of ozonesonde observations made in Huntsville, AL, during the peak ozone season (May to September) in 2013 indicate that ozone in the planetary boundary layer was significantly lower than the climatological average, especially in July and August when the Southeastern United States (SEUS) experienced unusually cool and wet weather. Because of a large influence of the lower stratosphere, however, upper tropospheric ozone was mostly higher than climatology, especially from May to July. Tropospheric ozone anomalies were strongly anticorrelated (or correlated) with water vapor (or temperature) anomalies with a correlation coefficient mostly about 0.6 throughout the entire troposphere. The regression slopes between ozone and temperature anomalies for surface up to midtroposphere are within 3.0–4.1 ppbv K−1. The occurrence rates of tropospheric ozone laminae due to STT are ≥50% in May and June and about 30% in July, August, and September suggesting that the stratospheric influence on free-tropospheric ozone could be significant during early summer. These STT laminae have a mean maximum ozone enhancement over the climatology of 52 ± 33% (35 ± 24 ppbv) with a mean minimum relative humidity of 2.3 ± 1.7%.

Models severely overestimate surface ozone in the Southeast US during summertime and this overestimation has implications for the design of air quality regulations. We use the GEOS-Chem model to interpret ozone observations from aircraft (SEAC4RS), ozonesondes (SEACIONS), and surface sites (CASTNET) in August–September 2013. After correcting for a 30–50 % NOx emission overestimate in the US EPA National Emission Inventory, we find that the model is unbiased relative to aircraft observations below 1 km. However, surface observations of maximum daily 8-h average (MDA8) ozone are still biased high in the model (averaging 48 ± 9 ppb) compared to observations (40 ± 9 ppb). The low tail in the observations (MDA8 ozone

We validate the Ozone Monitoring Instrument (OMI) Ozone Profile (PROFOZ) product from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against ozonesonde observations. We also evaluate the effects of OMI row anomaly (RA) on the retrieval by dividing the dataset into before and after the occurrence of serious OMI RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). The retrieval shows good agreement with ozonesondes in the tropics and midlatitudes and for pressure ∼ 50 hPa after applying OMI averaging kernels to ozonesonde data. The MBs of the stratospheric ozone column (SOC, the ozone column from the tropopause pressure to the ozonesonde burst pressure) are within 2 % with SDs of ∼ 50 hPa. The SOC MBs increase up to 3 % with SDs as great as 6 % and the TOC SDs increase up to 30 %. The comparison generally degrades at larger solar zenith angles (SZA) due to weaker signals and additional sources of error, leading to worse performance at high latitudes and during the midlatitude winter. Agreement also degrades with increasing cloudiness for pressure > ∼ 100 hPa and varies with cross-track position, especially with large MBs and SDs at extreme off-nadir positions. In the tropics and midlatitudes, the post-RA comparison is considerably worse with larger SDs reaching 2 % in the stratosphere and 8 % in the troposphere and up to 6 % in TOC. There are systematic differences that vary with latitude compared to the pre-RA comparison. The retrieval comparison demonstrates good long-term stability during the pre-RA period but exhibits a statistically significant trend of 0.14–0.7 % year−1 for pressure

Lightning is a particularly significant NOx source in the middle and upper troposphere where it affects tropospheric chemistry and ozone. Because the version-4 Community Multiscale Air Quality Modeling System (CMAQ) does not account for NOx emission from lightning, it underpredicts NOx above the mixed layer. In this study, the National Lightning Detection Network™ (NLDN) lightning data are applied to the CMAQ model to simulate the influence of lightning-produced NOx (LNOx) on upper tropospheric NOx and subsequent ozone concentration. Using reasonable values for salient parameters (detection efficiency ∼95%, cloud flash to ground flash ratio ∼3, LNOx production rate ∼500 mol N per flash), the NLDN ground flashes are converted into total lightning NOx amount and then vertically distributed on 39 CMAQ model layers according to a vertical-distribution profile of lightning N mass. This LNOx contributes 27% of the total NOx emission during 15 July ∼7 September 2006. This additional NOx reduces the low-bias of simulated tropospheric O3 columns with respect to OMI tropospheric O3 columns from 10 to 5%. Although the model prediction of ozone in upper troposphere improves by ∼20 ppbv due to lightning-produced NOx above the southeastern and eastern U.S.A., the improved ozone prediction is still ∼20–25 ppbv lower than ozonesonde measurements.

This study evaluates source attribution of ozone (O3) in the southeast United States (US) within O3 lamina observed by the University of Alabama in Huntsville (UAH) Tropospheric Ozone Lidar Network (TOLNet) system during June 2013. This research applies surface-level and airborne in situ data and chemical transport model simulations (GEOS-Chem) in order to quantify the impact of North American anthropogenic emissions, wildfires, lightning NOx, and long-range/stratospheric transport on the observed O3 lamina. During the summer of 2013, two anomalous O3 layers were observed: (1) a nocturnal near-surface enhancement and (2) a late evening elevated (3–6 km above ground level) O3 lamina. A “brute force” zeroing method was applied to quantify the impact of individual emission sources and transport pathways on the vertical distribution of O3 during the two observed lamina. Results show that the nocturnal O3 enhancement on 12 June 2013 below 3 km was primarily due to wildfire emissions and the fact that daily maximum anthropogenic emission contributions occurred during these night-time hours. During the second case study it was predicted that above average contributions from long-range/stratospheric transport was largely contributing to the O3 lamina observed between 3 and 6 km on 29 June 2013. Other models, remote-sensing observations, and ground-based/airborne in situ data agree with the source attribution predicted by GEOS-Chem simulations. Overall, this study demonstrates the dynamic atmospheric chemistry occurring in the southeast US and displays the various emission sources and transport processes impacting O3 enhancements at different vertical levels of the troposphere.

This paper addresses several aspects related to ultraviolet (UV) measurements from an upcoming geostationary orbit (GEO) satellite mission. First, using simulated cloud coverage based on the MTSAT (Multi-functional Transport Satellite 1R) 650 nm channel as a proxy, we find that GEO observations can increase clear-sky coverage by ~ 4 times. Secondly, we examine the feasibility of improved ozone detection with GEO observations, using synthetic GEMS spectra with GEO geometries along with the TOMS total ozone algorithm and an ozone profile algorithm based on the optimal estimation method. The sensitivity of ozone retrievals to the lower troposphere is limited at large solar and satellite zenith angles, especially above 70° under clear-sky conditions. Third, we evaluate two new ideas for improving ozone retrieval sensitivity in the troposphere at large angle geometries; (1) a geosynchronous orbit with an inclination-angle of 30°, with smaller values of viewing zenith angles than those from a geostationary orbit; (2) a combination of UV measurements at multiple solar zenith angles to improve the accuracy of ozone profile retrievals.

We evaluate the Ozone Monitoring Instrument (OMI) ozone profile retrieval against ozonesonde data and the Environmental Protection Agency (EPA) surface measurements for August 2006. Comparison of individual OMI ozone profile with ozonesonde indicates that OMI ozone profile can explain the general vertical variation of ozone but is limited in observing the boundary layer ozone, due to weak sensitivity to boundary layer ozone and thick lowest layer (∼2.5 km). We made pair-wise comparison between OMI and ozonesondes on 24 OMI vertical layers, as well as the 39 sigma-P vertical layers of the Community Multi-scale Air Quality (CMAQ) modeling system, respectively. OMI shows reasonable agreement with ozonesonde in the lower- to mid-troposphere. In the upper troposphere, while the bias increases, the normalized bias does not show much variation and remains below 10%. Comparison with EPA’s surface-monitoring data indicates that OMI observations at the lowest layer (surface to 2.5 km altitude) represent the mean values. While OMI underestimates elevated ozone concentrations, it explains the larger-scale spatial variation seen in the surface monitors.

An ozone enhancement in the nocturnal residual layer was observed by the Huntsville ozone lidar from the late evening to midnight on 4 October 2008. The well-correlated ozone, aerosol, water vapor, and wind structures suggest a low-level jet is responsible for this ozone enhancement. HYSPLIT backward trajectories support this conclusion with southerly transport suggesting Birmingham, AL as the source. Correspondingly, the higher increasing rate of surface ozone observed in the morning of 5 October can be explained by the entrainment into the mixed layer of higher ozone aloft on this day as compared with 4 October. This case study demonstrates the importance of continuous high-resolution lidar profiling for capturing short-duration ozone variations in the lower troposphere. Published by Elsevier Ltd.

A tropospheric ozone Differential Absorption Lidar system, developed jointly by The University of Alabama in Huntsville and the National Aeronautics and Space Administration, is making regular observations of ozone vertical distributions between 1 and 8 km with two receivers under both daytime and nighttime conditions using lasers at 285 and 291 nm. This paper describes the lidar system and analysis technique with some measurement examples. An iterative aerosol correction procedure reduces the retrieval error arising from differential aerosol backscatter in the lower troposphere. Lidar observations with coincident ozonesonde flights demonstrate that the retrieval accuracy ranges from better than 10% below 4 km to better than 20% below 8 km with 750-m vertical resolution and 10-min temporal integration.

In collaboration with the Jefferson County Department of Health and the Environmental Protection Agency (EPA), the University of Alabama in Huntsville developed a novel sensor for detecting very low levels of volatile organic compounds (VOCs). This sensor uses a commercial Fourier-transform infrared (FTIR) spectrometer, a commercial long-path IR gas cell, a commercial acoustic Stirling cyrocooler, and a custom cryogen-free cryotrap to improve sensitivity in an autonomous system with on-board quality control and quality assurance. Laboratory and initial field results show this methodology is sensitive to and well-suited for a wide variety of VOC atmospheric research and monitoring applications, including EPA National Air Toxics Trends Stations and the National Core monitoring network.

A statistical ensemble of microphysical parameters of the background stratospheric aerosol at altitudes of 15 to 30 km is modeled on the basis of experimental data. The aerosol attenuation coefficients (AACs) in the wavelength range 0.38–16.3 μm are calculated for all realizations of the ensemble by algorithms of the Mie theory. Analysis of correlations between the AACs and the microphysical parameters indicate that the AAC correlates most strongly with the total volume V and area S of all particles. The errors of determining the microphysical parameters from AAC measurements are analyzed via the method of linear regression. It is shown that, if the AAC is measured with an error of 5%, the errors of determining both the particle size distribution (PSD) for particles with sizes of 0.4 to 4 μm and the parameter S are an order of magnitude smaller than the prior uncertainty, whereas the error of determining V is two orders of magnitude smaller than the prior uncertainty. Schemes of AAC measurements with the SAGE III, ISAMS, CLAES, HALOE instruments and an IR interferometer in the visible and IR regions are discussed. It is shown that combining the schemes makes it possible to extend the range of particle sizes for which the PSD is retrieved with a satisfactory accuracy and to increase the accuracy of determining S and V substantially and the accuracy of determining the total number of particles N opt to a lesser extent. Examples of interpreting AAC measurements carried out simultaneously with the SAGE III and HALOE instruments within the same spatial region are presented. A systematic discrepancy between vertical profiles of S and V obtained from SAGE III and HALOE measurements is revealed.

Two autonomous ozone measurement systems for use on ocean buoys and towers have been built and are discussed herein. They are based on low-power atmospheric ozone sensors from Physical Sciences Inc. (PSI) and 2B Technologies. The PSI sensor operates at 1 Hz with a precision of 1 ppb but requires about 45 W with the present data system; the 2B makes a measurement every 10 s with a precision of 1‐2 ppb and uses less than 4 W. The sensors have been packaged in watertight enclosures with a set of valves and filters to keep out seawater and aerosols. A controller uses data from the sensors and a meteorological system to determine whether sampling should proceed. If a sensor malfunction (such as an incorrect valve position or a temperature beyond its proper range) is detected, the controller attempts to correct it. Both sensors have been tested and used over the ocean, and one complete ozone measurement system (with the PSI sensor) has been successfully deployed on a buoy off Woods Hole, Massachusetts. In 2003, this system was operated at the Chesapeake Bay Lighthouse Tower for over a month with excellent results. The 2B system was also successfully tested in 2003 at a nearby offshore tower. The design of the systems and their testing and deployments are described, and data from some of the first experiments are presented.

Accurate remote sensing retrieval of atmospheric constituents over cloudy areas is very challenging because of insufficient knowledge of cloud parameters. Cloud treatments are highly idealized in most retrieval algorithms. Using a radiative transfer model treating clouds as scattering media, we investigate the effects of assuming opaque Lambertian clouds and employing a Partial Cloud Model (PCM) on Total Ozone Mapping Spectrometer (TOMS) ozone retrievals, especially for tropical high-reflectivity clouds. Assuming angularly independent cloud reflection is good because the Ozone Retrieval Errors (OREs) are within 1.5% of the total ozone (i.e., within TOMS retrieval precision) when Cloud Optical Depth (COD)⩾20. Because of Intra-Cloud Ozone Absorption ENhancement (ICOAEN), assuming opaque clouds can introduce large OREs even for optically thick clouds. For a water cloud of COD 40 spanning 2– 12 km with 20.8 Dobson Unit (DU) ozone homogeneously distributed in the cloud, the ORE is 17.8 DU in the nadir view. The ICOAEN effect depends greatly on solar zenith angle, view zenith angle, and intra-cloud ozone amount and distribution. The TOMS PCM is good because negative errors from the cloud fraction being underestimated partly cancel other positive errors. At COD⩽5, the TOMS algorithm retrieves approximately the correct total ozone because of compensating errors. With increasing COD up to 20–40, the overall positive ORE increases and is finally dominated by the ICOAEN effect. The ICOAEN effect is typically 5–13 DU on average over the Atlantic and Africa and 1–7 DU over the Pacific for tropical high-altitude (cloud top pressure ⩽300 hPa ) and high-reflectivity (reflectivity ⩾ 80%) clouds. Knowledge of TOMS ozone retrieval errors has important implications for remote sensing of ozone/trace gases from other satellite instruments.

This study investigates anomalous ozone distributions over cloudy areas in Nimbus-7 (N7) and Earth-Probe (EP) TOMS version-7 data and analyzes the causes for ozone anomaly formation. A 5°-longitude by 5°-latitude region is defined to contain a Positive Ozone Anomaly (POA) or Negative Ozone Anomaly (NOA) if the correlation coefficient between total ozone and reflectivity is > 0.5 or < -0.5. The average fractions of ozone anomalies among all cloud fields are 31.8 ± 7.7% and 35.8 ± 7.7% in the N7 and EP TOMS data, respectively. Some ozone anomalies are caused by ozone retrieval errors, and others are caused by actual geophysical phenomena. Large cloud-height errors are found in the TOMS version-7 algorithm in comparison to the Temperature Humidity Infrared Radiometer (THIR) cloud data. On average, cloud-top pressures are overestimated by ~200 hPa (THIR cloud-top pressure < 200 hPa) for high-altitude clouds and underestimated by ~150 hPa for low-altitude clouds (THIR cloud-top pressure > 750 hPa). Most tropical NOAs result from negative errors induced by large cloud-height errors, and most tropical POAs are caused by positive errors due to intra-cloud ozone absorption enhancement. However, positive and negative errors offset each other, reducing the ozone anomaly occurrence in TOMS data. Large ozone/reflectivity slopes for mid-latitude POAs show seasonal variation consistent with total ozone fluctuation, indicating that they result mainly from synoptic and planetary wave disturbances. POAs with an occurrence fraction of 30--60% occur in regions of marine stratocumulus off the west coast of South Africa and off the west coast of South America. Both fractions and ozone/reflectivity slopes of these POAs show seasonal variations consistent with that in the tropospheric ozone. About half the ozone/reflectivity slope can be explained by ozone retrieval errors over clear and cloudy areas. The remaining slope may result from there being more ozone production because of rich ozone precursors and higher photolysis rates over high-frequency, low-altitude clouds than in clear areas. Ozone anomalies due to ozone retrieval errors have important implications in TOMS applications such as tropospheric ozone derivation and analysis of ozone seasonal variation.

Using TOMS total-ozone measurements over high-altitude cloud locations and nearby paired clear locations, we describe the Clear-Cloudy Pairs (CCP) method for deriving tropical tropospheric ozone. The high-altitude clouds are identified by measured 380 nm reflectivities greater than 80% and Temperature Humidity InfraRed (THIR) measured cloud-top pressures less than 200 hPa. To account for locations without high-altitude clouds, we apply a zonal sine fitting to the stratospheric ozone derived from available cloudy points, resulting in a wave-one amplitude of about 4 DU. THIR data is unavailable after November 1984, so we extend the CCP method by using a reflectivity threshold of 90% to identify high-altitude clouds and remove the influence of high-reflectivity-but-low-altitude clouds with a lowpass frequency filter. We correct ozone retrieval errors associated with clouds, and ozone retrieval errors due to sun glint and aerosols. Comparing CCP results with Southern Hemisphere ADditional OZonesondes (SHADOZ) tropospheric ozone indicates that CCP tropospheric ozone and ozonesonde measurements agree, on average, to within 3 ± 1 DU standard error of the mean. The most significant difference between CCP and ozonesonde tropospheric ozone can be explained by the low Total Ozone Mapping Spectrometer (TOMS) version-7 retrieval efficiency of ozone in the lower troposphere.

The Atmospheric Infrared Sounder/Advanced Microwave Sounding Unit/Humidity Sounder for Brazil (AIRS/AMSU/HSB) instrument suite onboard Aqua observes infrared and microwave radiances twice daily over most of the planet. AIRS offers unprecedented radiometric accuracy and signal to noise throughout the thermal infrared. Observations from the combined suite of AIRS, AMSU, and HSB are processed into retrievals of atmospheric parameters such as temperature, water vapor, and trace gases under all but the cloudiest conditions. A more limited retrieval set based on the microwave radiances is obtained under heavy cloud cover. Before measurements and retrievals from AIRS/AMSU/HSB instruments can be fully utilized they must be compared with the best possible in situ and other ancillary "truth" observations. Validation is the process of estimating the measurement and retrieval uncertainties through comparison with a set of correlative data of known uncertainties. The ultimate goal of the validation effort is retrieved product uncertainties constrained to those of radiosondes: tropospheric rms uncertainties of 1.0 degC over a 1-km layer for temperature, and 10% over 2-km layers for water vapor. This paper describes the data sources and approaches to be used for validation of the AIRS/AMSU/HSB instrument suite, including validation of the forward models necessary for calculating observed radiances, validation of the observed radiances themselves, and validation of products retrieved from the observed radiances. Constraint of the AIRS product uncertainties to within the claimed specification of 1 K/1 km over well-instrumented regions is feasible within 12 months of launch, but global validation of all AIRS/AMSU/HSB products may require considerably more time due to the novelty and complexity of this dataset and the sparsity of some types of correlative observations.

Motivated by the desire to accurately derive tropospheric ozone from Total Ozone Mapping Spectrometer (TOMS) measurements, we investigate several aspects of these observations in the presence of highly reflecting clouds. Using the collocated Temperature Humidity InfraRed (THIR) measurements of cloud-top pressures, we identify three TOMS algorithm errors resulting from the inaccurate assignment of cloud-top pressure. The most significant error results from the inappropriate tropospheric ozone amount added below cloudy scenes to complete the total ozone column. After accounting for the cloud-height errors, we find significant total ozone column excesses of 10–15 Dobson units (DU) (1 DU = 2.6867×1016 molecules cm−2) over high-altitude, highly reflecting clouds compared with clear area observations. After accounting for additional algorithm errors involving the tropospheric ozone climatology and considering potential dynamical, photochemical, and NIMBUS-7/Earth Probe calibration errors, approximately 4–9 DU excesses over cloudy scenes remain. We speculate that the TOMS algorithm approximation of clouds as opaque Lambertian reflecting surfaces may account for a significant portion of these unexplained excesses. The excess ozone due to calibration error and unknown sources will affect the tropospheric ozone derived from TOMS measurements using clear/cloudy difference techniques.

Using Total Ozone Mapping Spectrometer (TOMS) version-7 level-2 clear-sky (reflectivity ≤ 20%) ozone measurements corrected for aerosol effects and sea-glint errors, we derived Lower Tropospheric Ozone (LTO) west and east of the Andes, the Mexican and Rocky Mountains, the mountains in Africa and the Arabian Peninsula, New Guinea, and the Himalayan Mountains. The derived results agree reasonably well with the seasonality of LTO from ozonesonde observations at Boulder, Cristobal, Fiji, Java, and Tahiti. The LTO seasonality found in the biomass burning seasons characterized by the ATSR World Fire Atlas west and east of the Andes (23°S–2°N), east of the Mexican Mountains (15°–23°N), South Sudan (6°–14°N), South Africa (30°–28°S), and west of New Guinea is consistent with the influence of biomass burning on the formation of tropospheric ozone in these regions. The significant El Nino influence on LTO west of New Guinea is evident throughout several El Nino cycles. The spring maximum in ozone west of the Mexican Mountains, in western China, and west of the Andes (32°–23°S) is consistent with a stratospheric intrusion source. East of the Mexican Mountains (23°–30°N), both west and east of the Rocky Mountains, in north Sudan and Iraq, and in western China, high concentrations of ozone are found in these continental and coastal regions which are affected by anthropogenic sources. The maximum ozone in these regions usually occurs in the summer due to photochemical ozone production. A summer LTO minimum occurs in coastal regions west of the Andes and west of Mexico, due to ozone destruction in low NOx and high H2O marine environment. A summer minimum also occurs in south Sudan in the rainy season. The LTO in the northern tropics of South America (4°–10°N), Africa (1°S–2°N), and east of New Guinea (7°–3°S) experiences little seasonal variation.

A series of ozone transects measured each year from 1987 to 1990 over thewestern Pacific and eastern Indian oceans between mid-November andmid-Decembershows a prominent ozone maximum reaching 50–80 ppbv between 5 and 10 kmin the 20° S–40° S latitude band. This maximum contrasts with ozonemixing ratios lower than20 ppbv measured at the same altitudes in equatorial regions. Analyses witha globalchemical transport model suggest that these elevated ozone values are part ofa large-scale tropospheric ozone plume extending from Africa to the western Pacific acrosstheIndian ocean. These plumes occur several months after the peak in biomassburninginfluence and during a period of high lightning activity in the SouthernHemispheretropical belt. The composition and geographical extent of these plumes aresimilar to theozone layers previously encountered during the biomass burning season in thisregion.Our model results suggest that production of nitrogen oxides from lightningstrokes sustains the NOx (= NO+NO2) levels and the ozonephotochemical productionrequired in the upper troposphere to form these persistent elevated ozonelayers emanating from biomass burning regions.

The time series of differences in coincident measurements of ozone by Stratospheric Aerosol and Gas Experiment (SAGE) and by Solar Backscattered Ultraviolet (SBUV), SBUV/2, Umkehr and Microwave Limb Sounder (MLS) are analyzed, and the slopes in the differences are calculated. SAGE ozone measurements are also compared against those by HALOE. The purpose of these comparisons is to look for statistically significant nonzero slopes which could indicate long-term calibration problems in one or more of the measurement systems. It is found that the slopes are remarkably similar between the Northern and Southern Hemisphere midlatitudes, and, apart from a few exceptions, the slopes are also similar in the tropics. Slopes of MLS-SAGE differences and HALOE-SAGE trends from approximately 1992 to 1996 have values of approximately -0.5 +/- 0.4%/yr (95% confidence limits) in Umkehr layers 7-9 (which are centered at approx. 37, 42, and 47 km altitude). Umkehr-SAGE slopes for 1979-1996, however, are almost all positive and in the range -0.1 - 0.41%/yr for Umkehr layers 4 - 8, while SBUV-SAGE slopes for 1979-1989 are essentially zero in layers 4 - 7 and 0.3-0.4%/yr in layers 8 and 9. Averaging all these results with SBUV-SAGE 11 slopes from 1985 to 1989, the other sensors minus SAGE slopes are most likely between 0.2 and -0.2%/yr1 from approx. 20 to 40 km altitude. The results indicate slightly negative slopes in Umkehr layers 5-7 and positive slopes in the other three layers. There thus appears to be no overall drift in the SAGE ozone measurements from 1979 to 1996, but SAGE sunrise/sunset trend differences greater than 40 km altitude, combined with the more accurate SBUV-SAGE slopes for 1979-1989, suggest a most likely slope range of 0.4 to -0.4%/yr between 40 and 50 km altitude. SBUV/2 measurements from 1989 to 1994 have an upward trend with respect to SAGE measurements of approx. 0.7% /yr with some altitudinal structure; this slope exceeds the estimated 95% uncertainties on the SBUV/2 trends.

Observations inside the November 1994 Antarctic stratospheric vortex and inside the April 1993 remnant Arctic stratospheric vortex by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer are reported. In both instances, elevated volume mixing ratios (VMRS) of carbon monoxide (CO) were measured. A peak Antarctic CO VMR of 60 ppbv (where 1 ppbv = 10(exp -9) per unit Volume) was measured at a potential temperature of 710 K (about 27 km), about 1 km below the altitude of a pocket of elevated NO(y) (total reactive nitrogen) at a deep minimum in N2O (

Vertical profiles of infrared cirrus extinction have been derived from tropical and subtropical upper tropospheric solar occultation spectra. The measurements were recorded by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the Atmospheric Laboratory for Applications and Sciences (ATLAS) 3 shuttle flight in November 1994. The presence of large numbers of small ice crystals is inferred from the appearance of broad extinction features in the 8-12 micron region. These features were observed near the tropopause and at lower altitudes. Vertical profiles of the ice extinction (/km) in microwindows at 831, 957, and 1204/cm have been retrieved from the spectra and analyzed with a model for randomly oriented spheroidal ice crystals. An area-equivalent spherical radius of 6 gm is estimated from the smallest ice crystals observed in the 8-12 micron region. Direct penetration of clouds into the lower stratosphere is inferred from observations of cloud extinction extending from the upper troposphere to 50 mbar (20 km altitude). Cloud extinction between 3 and 5 micron shows very little wavelength dependence, at least for the cases observed by the ATMOS instrument in the tropics and subtropics during ATLAS 3.

Ground-based lidars are suitable for long-term ozone monitoring as a complement to satellite and ozonesonde measurements. However, current ground-based lidars are unable to consistently measure ozone below 500 m above ground level (AGL) due to both engineering issues and high retrieval sensitivity to various measurement errors. In this paper, we present our instrument design, retrieval techniques, and preliminary results that focus on the high-temporal profiling of ozone within the atmospheric boundary layer (ABL) achieved by the addition of an inexpensive and compact mini-receiver to the previous system. For the first time, to the best of our knowledge, the lowest, consistently achievable observation height has been extended down to 125 m AGL for a ground-based ozone lidar system. Both the analysis and preliminary measurements demonstrate that this lidar measures ozone with a precision generally better than ±10% at a temporal resolution of 10 min and a vertical resolution from 150 m at the bottom of the ABL to 550 m at the top. A measurement example from summertime shows that inhomogeneous ozone aloft was affected by both surface emissions and the evolution of ABL structures.