Understanding ozone episodes during the TRACER-AQ campaign in Houston, Texas: The role of transport and ozone production sensitivity to precursors
Explore the source record for details and available documents.
54 ENVIRONMENTAL SCIENCES↗
SEARCH · Search NASA
Results for “OZONE”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Chemical changes in thirdhand smoke associated with remediation using an ozone generator
Ozonation is a common remediation approach to eliminate odors from mold, tobacco and fire damage in buildings. Little information exists to: 1) assess its effectiveness; 2) provide guidance on operation conditions; and 3) identify potential risks associated with the presence of indoor ozone and ozonation byproducts. The goal of this study is to evaluate chemical changes in thirdhand smoke (THS) aerosols induced by high levels of ozone, in comparison with THS aerosols aged under similar conditions in the absence of ozone. Samples representing different stages of smoke aging in the absence of ozone, including freshly emitted secondhand smoke (SHS) and THS, were collected inside an 18-m 3 room-sized chamber over a period of 42 h after six cigarettes were consumed. The experiments involved collection and analysis of gas phase species including volatile organic compounds (VOCs), volatile carbonyls, semivolatile organic compounds (SVOCs), and particulate matter. VOC analysis was carried out by gas chromatography/mass spectrometry with a thermal desorption inlet (TD-GC/MS), and volatile carbonyls were analyzed by on-line derivatization with dinitrophenylhydrazine (DNPH), followed by liquid chromatography with UV/VIS detection. SVOCs were extracted from XAD-coated denuders and Teflon-coated fiberglass filters in the absence of ozone. In those extracts, tobacco-specific nitrosamines (TSNAs) and other SVOCs were analyzed by gas chromatography with positive chemical ionization-triple quadrupole mass spectrometric detection (GC/PCI-QQQ-MS), and polycyclic aromatic hydrocarbons (PAHs) were quantified by gas chromatography with ion trap mass spectrometric detection (GC/IT-MS) in selected ion monitoring mode. Particulate matter concentration was determined gravimetrically. In a second experiment, a 300 mg h -1 commercial ozone generator was operated during 1 h, one day after smoke was generated, to evaluate the remediation of THS by ozonation. VOCs and volatile carbonyls were analyzed before and after ozonation. Extracts from fabrics that were exposed in the chamber before and after ozonation as surrogates for indoor furnishings were analyzed by GC/IT-MS, and aerosol size distribution was studied with a scanning mobility particle sizer. Ozone concentration was measured with a photometric detector. An estimated 175 mg ozone reacted with THS after 1 h of treatment, corresponding to 58% of the total O 3 released during that period. Fabric-bound nicotine was depleted after ozonation, and the surface concentration of PAHs adsorbed to fabric specimens decreased by an order of magnitude due to reaction with ozone, reaching pre-smoking levels. These results suggest that ozonation has the potential to remove harmful THS chemicals from indoor surfaces. However, gas phase concentrations of volatile carbonyls, including formaldehyde, acetaldehyde and acetone were higher immediately after ozonation. Ultrafine particles (UFP, in most cases with size <60 nm) were a major ozonation byproduct. UFP number concentrations peaked shortly after ozonation ended, and remained at higher-than background levels for several hours. Based on these results, minimum re-entry times after ozone treatment were predicted for different indoor scenarios. Clearly defining re-entry times can serve as a practical measure to prevent acute exposures to ozone and harmful ozonation byproducts after treatment. This study evaluated potential benefits and risks associated with THS remediation using ozone, providing insights into this technology.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Evaluating Diurnal Ozone Emissions: A Comparative Analysis of DSCOVR EPIC, PANDORA, and TOLNet Data for Space-Based Monitoring Assessment: A Case Study by ASDC
Stratospheric ozone occurs naturally in the upper atmosphere, forming a protective layer that shields us from the sun's harmful ultraviolet rays. Tropospheric ozone is not emitted directly into the air but is created by chemical reactions between nitrogen oxides (NOx) and volatile organic compounds (VOC). This reaction happens when pollutants emitted by cars, power plants, industrial boilers, refineries, chemical plants, and other sources chemically react in sunlight [1]. Therefore, increased levels of tropospheric ozone indicate the presence of pollutants in the air. While daily anthropogenic activity causes an increase of ground-level ozone, variation of stratospheric ozone changes happens much slower, so that variation of the total ozone column reflects the variation of the tropospheric column due to natural, e.g., wildfires and anthropogenic air pollution. Both total and tropospheric ozone column products are used in this study. The reflectance spectra measured by the Earth Polychromatic Imaging Camera (EPIC) instrument aboard the Deep Space Climate Observatory (DSCOVR) spacecraft are compared with a set of radiative transfer-derived lookup tables for the EPIC filter transmission functions and a wide range of ozone values to retrieve ozone with a maximum resolution of 18 km at the sub-satellite point [2]. EPIC provides total column ozone in level 2 and level 4 products and tropospheric column ozone in level 4 products. Both EPIC Ozone products [2] are available at the Atmospheric Science Data Center (ASDC) at NASA Langley Research Center [3, 4]. Pandora spectrometer instrument measures columnar amounts of trace gases in the atmosphere. These gases (O3, NO2, CH2O) absorb light from the sun at specific wavelengths in the ultraviolet-visible spectrum [5]. Using the theoretical solar spectrum as a reference, Pandora determines trace gas amounts using differential optical absorption spectroscopy (DOAS). Pandora ozone retrievals are available from the Pandonia Global Network [6]. Pandora data from North American major metropolitan areas, New York, NY, Washington DC, Los Angeles, CA, and Mexico City. Tropospheric Ozone Lidar Network (TOLNet) was established in 2012 to provide high spatiotemporal observations of tropospheric ozone to (1) better understand physical processes driving the ozone budget in various meteorological and environmental conditions and (2) validate the tropospheric ozone measurements of space-borne missions [7]. TOLNet data are available at ASDC [8]. While EPIC provides global coverage of ozone retrievals several times daily, temporal resolution may miss some features in daily ozone variations. Ground-based sensors such as Pandora spectrometers and TOLNet lidars provide better temporal resolution while missing continuous spatial coverage. The forthcoming ozone retrieval from the TEMPO mission [9] will provide better spatial and temporal coverage of air quality (including ozone) over North America. This study investigates whether EPIC ozone products can detect diurnal air quality variations and compare ozone temporal development with retrieval by ground-based instruments.
diurnal ozone emissions, DSCOVR EPIC, PANDORA, spa↗
Stratospheric Impact on the Northern Hemisphere Winter and Spring Ozone Interannual Variability in the Troposphere
In this study we use ozone and stratospheric ozone tracer simulations from the high-resolution (0.5°x0.5°) Goddard Earth Observing System, Version 5 (GEOS-5) in a replay mode to study the impact of stratospheric ozone on tropospheric ozone interannual variability (IAV). We use these simulations in conjunction with ozone sonde measurements from 1990 to 2016 during the winter and spring seasons. The simulations include a stratospheric ozone tracer (StratO3) to aid 15in the evaluation of the impact of stratospheric ozone IAV on the IAV of tropospheric ozone at different altitudes and location. The model is in good agreement with the observed interannual variation of tropospheric ozone, except for the post-Pinatubo period(1992-1994)over the region of North America. Ozone sonde data show a negative ozone anomaly in 1992-1994 following the Pinatubo eruption, with recovery thereafter. The simulated anomaly is only half the magnitude of that observed. Our analysis suggests that the simulated Stratosphere-troposphere exchange (STE)flux deduced from the analysis 20might be too strong over the North American (50°N-70°N) region after the Mt. Pinatubo eruption in the early 1990s,maskingthe impact of lower stratospheric ozone concentration on tropospheric ozone. European ozone sonde measurements show a similar but weaker ozone depletion after the Mt. Pinatubo eruption, which is fully reproduced by the model. Analysis based on the stratospheric ozone tracer (StratO3) identifies differences in strength and vertical extent of stratospheric ozone impact on the tropospheric ozone interannual variation (IAV)between North America and Europe. Over NorthAmerica25stations, the StratO3IAV has a significant impact on tropospheric ozone from the upper to lower troposphere and explains about 60% and 66% of the simulated ozone IAV at 400 hPa, and ~11% and 34% at 700 hPa in winter and spring respectively. Over European stations, the influence is limited to the middle to upper troposphere, and becomes much smaller at 700 hPa. The Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2)assimilated fields exhibit strong longitudinal variations over northern hemisphere (NH) mid-high latitudes, with lower tropopause height and 30lower geopotential height over North America than Europe. These variations associated with the relevant variations in the location of tropospheric jet flows are responsible for the longitudinal differences in the stratospheric ozone impact, with stronger effects over North America than over Europe
tropospheric ozone IAV, Model, ozonesonde, stratos↗
On the Quality of the Nimbus 7 LIMS Version 6 Ozone for Studies of the Middle Atmosphere
The Nimbus 7 Limb Infrared Monitor of the Stratosphere (LIMS) radiance profile dataset of 1978/79 was reconditioned and reprocessed to Version 6 (V6) profiles of temperature and species that are improved significantly over those from Version 5 (V5). The LIMS V6 dataset was archived for public use in 2002. Improvements for its ozone include: (1) a more accurate accounting for instrument and spacecraft motion effects in the radiances, (2) the use of better spectroscopic line parameters for its ozone forward model, (3) retrievals of all its scans, (4) more accurate and compatible temperature versus pressure profiles (or T(p)), which are needed for the registration of the ozone radiances and for the removal of temperature effects from them, and (5) a better accounting for interfering species in the lower stratosphere. The retrieved V6 ozone profiles extend from near cloud top altitudes to about 80 km and from 64S to 84N latitude with better sampling along the orbit than for the V5 dataset. Calculated estimates of the single-profile precision and accuracy are provided for the V6 ozone from this study. Precision estimates based on the data themselves are of order 3% or better from 1 to 30 hPa. Estimates of total systematic error for a single profile are hard to generalize because the separate sources of error may not all be of the same sign and they depend somewhat on the atmospheric state. It is estimated that the V6 zonal mean ozone distributions are accurate to within 9% to 7% from 50 hPa to 3 hPa, respectively. Effects of a temperature bias can be significant and may be present at 1 to 2 hPa though. There may be ozone biases of order 10% at those levels due to possible biases of up to +2 K, but there is no indication of a similar problem elsewhere in the stratosphere. Simulation studies show that the LIMS retrievals are also underestimating slightly the small amplitudes of the atmospheric temperature tides, which affect its retrieved day/night ozone differences. There are small biases in the middle to lower stratosphere for the ascending versus descending node LIMS ozone, due principally to not accounting for the asymmetric weighting of its radiances across the tangent layer. The estimates of total accuracy were assessed by comparing the daily zonal mean LIMS ozone distributions against those from the Nimbus 7 SBUV Version 8 (V8) dataset for the same period. Generally, the LIMS V6 ozone agrees well with SBUV, except perhaps in the tropical lower stratosphere where the LIMS ozone is less. Still, the accuracy for LIMS V6 ozone in the lower stratosphere is improved over that found for LIMS V5, as indicated by several LIMS comparisons with ECC ozonesonde profiles. The LIMS V6 ozone is considered especially suitable for detailed studies of large-scale stratospheric processes above the 100-hPa level. Comparison of diurnal, photochemical model calculations with the monthly-averaged, upper stratospheric ozone observed from LIMS V6 indicates only a slight ozone deficit for the model at about 2 hPa. However, that deficit exhibits little to no seasonal variation and is in good agreement with similar model comparisons for a seasonal time series of ozone obtained with ground-based microwave instruments. Because the LIMS V6 ozone in the lower stratosphere has improved accuracy and sampling versus that of V5, it should now be possible to conduct quantitative studies of ozone transport and chemistry for the northern hemisphere, polar stratospheric winter of 1978/79 a time period when the catalytic loss of ozone due to reactive chlorine should not have been a major factor for the Arctic region.
Remsberg, Ellis↗
Monitoring of Observation Errors in the Assimilation of Satellite Ozone Data
The stratospheric ozone layer protects life on Earth from the harmful effects of solar ultravioiet radiation. The ozone layer is currently in a fragile state because of depletion caused by man-made chemicals, especially chlorofluorocarbons. The state of the ozone layer is being monitored and evaluated by scientific experts around the world, in order to help policy makers assess the impacts of international protocols that control the production and release of ozone depleting chemicals. Scientists use a variety ozone measurements and models in order to form a comprehensive picture about the current state of the ozone layer, and to predict the future behavior (expected to be a recovery, as the abundance of the depleting chemicals decreases). Among the data sets used, those from satellite-borne instruments have the advantage of providing a wealth of information about the ozone distribution over most of the globe. Several instruments onboard American and international satellites make measurements of the properties of the atmosphere, from which atmospheric ozone amounts are estimated; long-term measurement programs enable monitoring of trends in ozone. However, the characteristics of satellite instruments change in time. For example, the instrument lenses through which measurements are made may deteriorate over time, or the satellite orbit may drift so that measurements over each location are made later and later in the day. These changes may increase the errors in the retrieved ozone amounts, and degrade the quality of estimated ozone amounts and of their variability. Our work focuses on combining the satellite ozone data with global models that capture atmospheric motion and ozone chemistry, using advanced statistical techniques: this is known as data assimilation. Our method provides a three-dimensional global ozone distribution that is consistent with both the satellite measurements and with our understanding of processes (described in the models) that control ozone distribution. Through the monitoring of statistical properties of the agreement between the data and the model, this approach also enables us to detect changes in the quality of ozone data retrieved from satellite-borne instrument measurements. This paper demonstrates that calculations of the changes in satellite data quality, and the impact these changes on the estimates of the global ozone distribution, can assist in maintaining the uniform quality of the satellite ozone data throughout the lifetime of these instruments, thus contributing to our understanding of long-term ozone change.
Stajner, Ivanka↗
Tropospheric and stratospheric ozone from assimilation of Aura data
Ozone is an atmospheric trace gas with multiple impacts on the environment. Global ozone fields are needed for air quality predictions, estimation of the ultraviolet radiation reaching the surface, climate-radiation studies, and may also have an impact on longer-term weather predictions. We estimate global ozone fields in the stratosphere and troposphere by combining the data from EOS Aura satellite with an ozone model using data assimilation. Ozone exhibits a large temporal variability in the lower stratosphere. Our previous work showed that assimilation of satellite data from limb-sounding geometry helps constrain ozone profiles in that region. We assimilated ozone data from the Aura Microwave Limb Sounder (MLS) and the Ozone Monitoring Instrument (OMI) into the ozone system at NASA's Global Modeling and Assimilation Office (GMAO). Ozone is transported within a general circulation model (GCM) which includes parameterizations for stratospheric photochemistry, tropospheric chemistry, and a simple scheme for heterogeneous ozone loss. The focus of this study is on the representation of ozone in the lower stratosphere and tropospheric ozone columns. We plan to extend studies of tropospheric ozone distribution through assimilation of ozone data from the Tropospheric Emission Spectrometer (TES). Comparisons with ozone sondes and occultation data show that assimilation of Aura data reproduces ozone gradients and variability in the lower stratosphere well. We proceed by separating the contributions to temporal changes in the ozone field into those that are due to the model and those that are due to the assimilation of Aura data. The impacts of Aura data are illustrated and their role in the representation of ozone variability in the lower stratosphere and troposphere is shown.
Stajner, I.↗
Attribution of Stratospheric and Tropospheric Ozone Changes Between 1850 and 2014 in CMIP6 Models
We quantify the impacts of halogenated ozone-depleting substances (ODSs), greenhouse gases (GHGs), and short-lived ozone precursors on ozone changes between 1850 and 2014 using single-forcing perturbation simulations from several Earth system models with interactive chemistry participating in the Coupled Model Intercomparison Project Aerosol and Chemistry Model Intercomparison Project. We present the responses of ozone to individual forcings and an attribution of changes in ozone columns and vertically resolved stratospheric and tropospheric ozone to these forcings. We find that whilst substantial ODS-induced ozone loss dominates the stratospheric ozone changes since the 1970s, in agreement with previous studies, increases in tropospheric ozone due to increases in short-lived ozone precursors and methane since the 1950s make increasingly important contributions to total column ozone (TCO) changes. Increases in methane also lead to substantial extra-tropical stratospheric ozone increases. Impacts of nitrous oxide and carbon dioxide on stratospheric ozone are significant but their impacts on TCO are small overall due to several opposing factors and are also associated with large dynamical variability. The multi-model mean (MMM) results show a clear change in the stratospheric ozone trends after 2000 due to now declining ODSs, but the trends are generally not significantly positive, except in the extra-tropical upper stratosphere, due to relatively small changes in forcing over this period combined with large model uncertainty. Although the MMM ozone compares well with the observations, the inter-model differences are large primarily due to the large differences in the models' representation of ODS-induced ozone depletion.
Halogenated ozone-depleting substances↗
Ground Based, Millimeter Wave Measurement of Ozone in the Middle Atmosphere
There is a need for highly reliable measurements of stratospheric ozone. Policy makers worldwide concerned with public health rely oil a clear consensus from the scientific community as a basis for ozone-related environmental policy that has a significant impact oil national economies. Tile latest Such consensus was presented in WMO, and used in a 1999 meeting of the parties considering amendments to the Montreal Protocol oil Substances that Deplete the Ozone Layer. Tile scientific community, in turn, needs highly precise and accurate measurements of ozone levels, and small time derivatives of these levels, both in continued - development of its understanding of the physical and chemical processes involved and as clear evidence that these processes are occurring as stated. Over most of the world, changes in ozone levels are small. For example, over the heavily populated northern midlatitudes, the linearized rate of ozone decline is between 0.2% per year and 0.7% per year, depending on altitude. These values are small enough to make measurement requirements technically challenging. Data quality may suffer from imperfections in individual instruments. In one instance, early results from a satellite-borne ozone sensor were later found to be invalid because of calibration drift. Even in the absence of drift, tile absolute calibration of a new sensor may differ slightly from that of its predecessor in service. Most ozone remote sensing instruments operate at ultraviolet or infrared wavelengths where scattering from dust and aerosols must be taken into account; results from these systems may be or are affected following a major volcanic eruption, such as tile one at Mt. Pinatubo in 1991. Given these difficulties, a consensus of measurements from several independent systems is required to insure a reliable understanding of stratospheric ozone levels. Because of the above-described need for highly precise and accurate ozone measurements using several independent techniques, there was interest in developing several techniques which were known but not highly developed in the 1980's into systems capable of being used in ail operational manner to make measurements with the level of quality needed to-detect small trends in ozone levels. A ground-based microwave instrument capable of remotely sensing stratospheric ozone had been designed by tile Principal Investigator of the present project. This instrument was built at tile Millitech Corporation in South Deerfield, Massachusetts before tile present work began. (Funding for design and construction of the instrument came from sources other than the present grant.) Tile instrument measured the spectrum of one of the many emission lines produced by purely rotational transitions of ozone, one at a frequency of 110.8 GHz. The altitude distribution of ozone can. in principle, be retrieved from the details of the pressure-broadened spectrum of the ozone transition. However, the level of contamination of the spectral measurement by instrumentally induced artifacts must be very low in order to retrieve a ozone profile of useful quality from it. The Millitech instrument demonstrated spectral purity at ail adequate level, and there were promising ideas for instrumental improvements and for further development of the technique. The initial objectives of the present project, then, were to develop techniques for calibrating the Millitech instrument, to minimize artifacts in tile spectra it produces, to optimally retrieve ozone profiles from tile spectra, to test tile quality of the microwave profiles by comparing them with profiles obtained using several other, independent techniques over both short and periods of time, and to perform research using the ozone data gathered with the instrument.
Parrish, Alan↗
The Re-Analysis of Ozone Profile Data from a 41-Year Series of SBUV Instruments
In this study we present the validation of ozone profiles from a number of Solar Back Scattered Ultra Violet (SBUV) and SBUV/2 instruments that were recently reprocessed using an updated (Version 8.6) algorithm. The SBUV dataset provides the longest available record of global ozone profiles, spanning a 41-year period from 1970 to 2011 (except a 5-year gap in the 1970s) and includes ozone profile records obtained from the Nimbus-4 BUV and Nimbus-7 SBUV instruments, and a series of SBUV(/2) instruments launched on NOAA operational satellites (NOAA 09, 11, 14, 16, 17, 18, 19). Although modifications in instrument design were made in the evolution from the BUV instrument to the modern SBUV(/2) model, the basic principles of the measurement technique and retrieval algorithm remain the same. The long term SBUV data record allows us to create a consistent, calibrated dataset of ozone profiles that can be used for climate studies and trend analyses. In particular, we focus on estimating the various sources of error in the SBUV profile ozone retrievals using independent observations and analysis of the algorithm itself. For the first time we include in the metadata a quantitative estimate of the smoothing error, defined as the error due to profile variability that the SBUV observing system cannot inherently measure. The magnitude of the smoothing error varies with altitude, latitude, season and solar zenith angle. Between 10 and 1 hPa the smoothing errors for the SBUV monthly zonal mean retrievals are of the order of 1 %, but start to increase above and below this layer. The largest smoothing errors, as large as 15-20%, were detected in in the troposphere. The SBUV averaging kernels, provided with the ozone profiles in version 8.6, help to eliminate the smoothing effect when comparing the SBUV profiles with high vertical resolution measurements, and make it convenient to use the SBUV ozone profiles for data assimilation and model validation purposes. The smoothing error can also be minimized by combining layers of data, and we will discuss recommendations for this approach as well. The SBUV ozone profiles have been intensively validated against satellite profile measurements obtained from the Microwave Limb Sounders (MLS) (on board the UARS and AURA satellites), Stratospheric Aerosol and Gas Experiment (SAGE) and Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). Also, we compare coincident and collocated SBUV ozone retrievals with observations made by ground-based instruments, such as microwave spectrometers, lidars, Umkehr instruments and balloon-borne ozonosondes. Finally, we compare the SBUV ozone profiles with output from the NASA GSFC GEOS-CCM model. In the stratosphere between 25 and 1 hPa the mean biases and standard deviations are within 5% for monthly mean ozone profiles. Above and below this layer the vertical resolution of the SBUV algorithm decreases and the effects of vertical smoothing should be taken into account. Though the SBUV algorithm has a coarser vertical resolution in the lower stratosphere and troposphere, it is capable of precisely estimating the integrated ozone column between the surface and 25 hPa. The time series of the tropospheric - lower stratospheric ozone column derived from SBUV agrees within 5% with the corresponding values observed by an ensemble of ozone sonde stations in North Hemisphere. Drift of the ozone time series obtained from each SBUV(/2) instrument relative to ground based and satellite measurements are evaluated and some features of individual SBUV(l2) instruments are discussed. In addition to evaluating individual instruments against independent observations, we also focus on the instrument to instrument consistency in the series. Overall, Version 8.6 ozone profiles obtained from two different SBUV(l2) instruments compare within a couple of percent during overlap periods and are consistently varying in time, with some exceptions. Some of the noted discrepancies might bssociated with ozone diurnal variations, since the difference in the local time of the observations for a pair of SBUV(l2) instruments could be several hours. Other issues include the potential short-term drift in measurements as the instrument orbit drifts, and measurements are obtained at high solar zenith angles (>85 ). Based on the results of the validation, a consistent, calibrated dataset of SBUV ozone profiles has been created based on internal calibration only.
Kramarova, Natalya↗
Retrieval of Ozone Column Content from Airborne Sun Photometer Measurements During SOLVE II: Comparison with SAGE III, POAM III,THOMAS and GOME Measurements
During the Second SAGE 111 Ozone Loss and Validation Experiment (SOLVE II), the 14- channel NASA Ames Airborne Trackmg Sunphotometer (AATS-14) was mounted on the NASA DC-8 and successfully 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 data by using a linear least squares method. For each AATS-14 measured TOD spectrum, this method iteratively finds the ozone column content that yields the best match between measured and calculated TOD. The calculations assume the known Chappuis ozone band shape and a three-parameter AOD shape (quadratic in log-log space). Seven of the AATS-14 channels (each employing an interference filter with a nominal full-width at half maximum bandpass of -5 nm) are within the Chappuis band, with center wavelengths between 452.9 nm and 864.5 nm. One channel (604.4 nm) is near the peak, and three channels (499.4, 519.4 and 675.1 nm) have ozone absorption within 30-40% of that at the peak. For the typical DC-8 SOLVE II cruising altitudes of approx. 8-12 km and the background stratospheric aerosol conditions that prevailed during SOLVE 11, absorption of incoming solar radiation by ozone comprised a significant fraction of the aerosol-plus-ozone optical depth measured in the four AATS-14 channels centered between 499.4 and 675.1 nm. Typical AODs above the DC-8 ranged from 0.003-0.008 in these channels. For comparison, an ozone overburden of 0.3 atm-cm (300 DU) translates to ozone optical depths of 0.009,0.014, 0.041, and 0.012, respectively, at these same wavelengths. In this paper, we compare AATS-14 values of ozone column content with temporally and spatially near-coincident values derived from measurements acquired by the Stratospheric Aerosol and Gas Experiment III (SAGE III) and the Polar Ozone and Aerosol Measurement 111 (POAM III) satellite sensors. We also compare AATS-14 ozone retrievals during selected DC-8 latitudinal and longitudinal 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 this comparison, the amount of ozone in the column below the aircraft is estimated by combining SAGE and/or POAM data with high resolution, fast response in-situ ozone measurements acquired during the DC-8 ascent at the start of each science flight.
Livingston, J.↗
Sensitivity of the Assimilated Ozone in the UTLS to Model and Data Selection Changes
This presentation will discuss the sensitivity of assimilated ozone fields in the upper troposphere and lower stratosphere (UTLS) to a number of factors, focusing mainly on aspects of data selection and the prediction model. This is important, because assimilation represents an attempt to construct our best estimates of the true ozone field; however, inaccuracies in the UTLS ozone distribution translate into an uncertainty in factors such as the calculated radiative forcing of climate or the inferred stratosphere-troposphere exchange (STE) of ozone. The 3D ozone data assimilation system, from NASA's Global Modeling and Assimilation Office (GMAO), combines observations of total ozone column and stratospheric profiles with predictions from an off-line, parameterized chemistry and transport model (pCTM) to produce six-hourly, global analyses. The first experiments discussed assimilate ozone retrievals from the Earth-Probe Total Ozone Mapping Spectrometer (EPTOMS) and stratospheric profiles from the Solar Backscatter UltraViolet/2 (SBUV/2) instrument. The SBUV/2 ozone data have a coarse vertical resolution, with increased uncertainty below the ozone maximum, and TOMS provides only total ozone columns. Thus, the assimilated ozone profiles in the UTLS region are only weakly constrained by the incoming SBUV and TOMS data. Consequently, the assimilated ozone distribution should be sensitive to changes in inputs to the statistical analysis scheme. Sensitivity studies have been conducted to examine the responses to TOMS and SBUV/2 data selection, modifications of the forecast and observation error covariance models, and the model formulation (turning off chemistry or using different wind analyses in the pCTM). The second set of experiments includes an additional data type: ozone retrieved from infrared limb-emission by MIPAS on Envisat. These data offer not only improved vertical resolution in the stratosphere, but also give measurements in the polar night. Comparisons of the assimilated ozone fields from both sets of experiments with independent observations, primarily ozone sondes, are used to determine the impact of each of these changes. It is shown that many of the changes have a significant impact on the UTLS ozone estimates. Implications for interpretation of STE and radiative forcing of climate are discussed.
Pawson, Steven↗
Assimilation of MLS and OMI Ozone Data
Ozone data from Aura Microwave Limb Sounder (MLS) and Ozone Monitoring Instrument (OMI) were assimilated into the ozone model at NASA's Global Modeling and Assimilation Office (GMAO). This assimilation produces ozone fields that are superior to those from the operational GMAO assimilation of Solar Backscatter Ultraviolet (SBUV/2) instrument data. Assimilation of Aura data improves the representation of the "ozone hole" and the agreement with independent Stratospheric Aerosol and Gas Experiment (SAGE) III and ozone sonde data. Ozone in the lower stratosphere is captured better: mean state, vertical gradients, spatial and temporal variability are all improved. Inclusion of OMI and MLS data together, or separately, in the assimilation system provides a way of checking how consistent OMI and MLS data are with each other, and with the ozone model. We found that differences between OMI total ozone column data and model forecasts decrease after MLS data are assimilated. This indicates that MLS stratospheric ozone profiles are consistent with OMI total ozone columns. The evaluation of error characteristics of OMI and MLS ozone will continue as data from newer versions of retrievals becomes available. We report on the initial step in obtaining global assimilated ozone fields that combine measurements from different Aura instruments, the ozone model at the GMAO, and their respective error characteristics. We plan to use assimilated ozone fields in estimation of tropospheric ozone. We also plan to investigate impacts of assimilated ozone fields on numerical weather prediction through their use in radiative models and in the assimilation of infrared nadir radiance data from NASA's Advanced Infrared Sounder (AIRS).
Stajner, I.↗
Interactive Ozone and Methane Chemistry in GISS-E2 Historical and Future Climate Simulations
The new generation GISS climate model includes fully interactive chemistry related to ozone in historical and future simulations, and interactive methane in future simulations. Evaluation of ozone, its tropospheric precursors, and methane shows that the model captures much of the largescale spatial structure seen in recent observations. While the model is much improved compared with the previous chemistry-climate model, especially for ozone seasonality in the stratosphere, there is still slightly too rapid stratospheric circulation, too little stratosphere-to-troposphere ozone flux in the Southern Hemisphere and an Antarctic ozone hole that is too large and persists too long. Quantitative metrics of spatial and temporal correlations with satellite datasets as well as spatial autocorrelation to examine transport and mixing are presented to document improvements in model skill and provide a benchmark for future evaluations. The difference in radiative forcing (RF) calculated using modeled tropospheric ozone versus tropospheric ozone observed by TES is only 0.016W/sq. m. Historical 20th Century simulations show a steady increase in whole atmosphere ozone RF through 1970 after which there is a decrease through 2000 due to stratospheric ozone depletion. Ozone forcing increases throughout the 21st century under RCP8.5 owing to a projected recovery of stratospheric ozone depletion and increases in methane, but decreases under RCP4.5 and 2.6 due to reductions in emissions of other ozone precursors. RF from methane is 0.05 to 0.18W/ sq. m higher in our model calculations than in the RCP RF estimates. The surface temperature response to ozone through 1970 follows the increase in forcing due to tropospheric ozone. After that time, surface temperatures decrease as ozone RF declines due to stratospheric depletion. The stratospheric ozone depletion also induces substantial changes in surface winds and the Southern Ocean circulation, which may play a role in a slightly stronger response per unit forcing during later decades. Tropical precipitation shifts south during boreal summer from 1850 to 1970, but then shifts northward from 1970 to 2000, following upper tropospheric temperature gradients more strongly than those at the surface.
Ozone↗
The threee-dimensional morphology of the Antarctic ozone hole
The three-dimensional morphology of the spring antarctic ozone distribution as determined by the Nimbus 7 Solar Backscatter Ultraviolet (SBUV) spectrometer instrument is presented for the period 1 to 11 October in 1986. The data show that a clearly defined minimum in ozone relative to the local ozone field extends throughout the stratosphere from the tropopause to above 50 km, though decreasing in intensity with altitude. Near 18 km ozone in the ozone hole is 50 percent less than the average surrounding ozone. But even at 50 km the ozone is 20 percent less than the surrounding ozone field. The ozone minimum in the upper stratosphere is displaced about 6 degrees toward the equator so that observations at a fixed station may provide the illusion that the ozone minimum is restricted only to low altitudes. While the ozone minimum is spatially coherent throughout the stratosphere, there are differences in the behavior of ozone at different altitudes that suggest the existence of at least three distinct altitude domains. Below 30 km ozone is characterized by classic ozone hole behavior. Between 33 and 43 km ozone is more stable, actually increasing during September and October. Above 43 km ozone has always decreased during September to a minimum in October, but it has suffered a long term decrease of 7 to 12 percent since 1979 similar to that seen at low altitudes.
Aikin, Arthur C.↗
Ozone Budgets from a Global Chemistry/ Transport Model and Comparison to Observations from POLARIS
The objective of the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) field mission was to obtain data to better characterize the summertime seasonal decrease of ozone at mid to high latitudes. The decrease in ozone occurs mainly in the lower stratosphere and is expected to result from in situ chemical destruction. Instrumented balloons and aircraft were used in POLARIS, along with satellites, to measure ozone and chemical species which are involved with stratospheric ozone chemistry. In order to close the seasonal ozone budget, however, ozone transport must also be estimated. Comparison to a global chemistry and transport model (CTM) of the stratosphere indicates how well the summertime ozone loss processes are simulated and thus how well we can predict the ozone response to changing amounts of chemical source gases. Moreover, the model gives insight into the possible relative magnitude of transport contributions to the seasonal ozone decline. Initial comparison to the Goddard CTM, which uses transport winds and temperatures from meteorological data assimilation, shows a high ozone bias in the model and an attenuated summertime ozone loss cycle. Comparison of the model chemical partitioning, and ozone catalytic loss rates to those derived from measurements shows fairly close agreement both at ER-2 altitudes (20 km) and higher. This suggests that the model transport is too active in resupplying ozone to the high latitude region, although chemistry failings cannot be completely ruled out. Comparison of ozone and related species will be shown along with a full diagnosis of the model ozone budget and its possible sources of error.
Kawa, S. Randy↗
History of Ozone Research: From Schonbein to the Present
In 1840, C.F. Schonbein recognized that the smell generated in several different electrical and chemical processes was a single substance. He named this substance "ozein" from the Greek for "to smell". This substance we know today as ozone. Several periods can be distinguished in the continued development of our understanding of ozone. Throughout the late 19th century, the identity and properties of ozone were established and described. Ozone was recognized to be a constituent of normal air and tests were established to measure its concentration. Its disinfectant properties were recognized. New methods were developed for making ozone in the laboratory. In 1879, ultraviolet spectroscopic techniques were applied to the measurement of the solar spectrum and it was discovered by Comu that the spectrum was cut off at about 300 nm wavelength. Hartley suggested, based on laboratory measurements, that this cutoff was due to ozone in the atmosphere which he correctly asserted was somewhere in the upper atmosphere. This began the period of development of the amount and distribution of ozone throughout the atmosphere. In 1930, Chapman put forward the first theory of the formation and destruction of ozone. By the mid-1960s it was becoming obvious that the description of the chemical loss term was inadequate. By the early 1970s the chemical destruction of ozone by the oxides of hydrogen, nitrogen, chlorine, and bromine was recognized as an essential element in the chemical balance determining the ozone concentration. Today, ozone is a broad research project which crosses the boundaries of traditional disciplines. Stratospheric ozone loss due to chlorofluorocarbons is a newsworthy item. The Antarctic ozone hole opens up every spring. The provisions of the Montreal Protocol were agreed upon by countries around the world and promise to reduce the future levels of ozone-destroying chlorine in the stratosphere. Ozone concentrations in polluted cities are a subject of local and national regulations to limit its potential for causing health problems and corrosive effects on materials. A lot is known about ozone but many new questions are still being developed.
Stolarski, Richard S.↗
Constructing Synoptic Maps of Stratospheric Column Ozone from HALOE, SAGE and Balloonsonde Data Using Potential Vorticity Isentropic Coordinate Transformations
In this study we utilize potential vorticity - isentropic (PVI) coordinate transformations as a means of combining ozone data from different sources to construct daily, synthetic three-dimensional ozone fields. This methodology has been used successfully to reconstruct ozone maps in particular regions from aircraft data over the period of the aircraft campaign. We expand this method to create high-resolution daily global maps of profile ozone data, particularly in the lower stratosphere, where high-resolution ozone data are sparse. Ozone climatologies in PVI-space are constructed from satellite-based SAGE II and UARS/HALOE data, both of which-use solar occultation techniques to make high vertical resolution ozone profile measurements, but with low spatial resolution. A climatology from ground-based balloonsonde data is also created. The climatologies are used to establish the relationship between ozone and dynamical variability, which is defined by the potential vorticity (in the form of equivalent latitude) and potential temperature fields. Once a PVI climatology has been created from data taken by one or more instruments, high-resolution daily profile ozone field estimates are constructed based solely on the PVI fields, which are available on a daily basis from NCEP analysis. These profile ozone maps could be used for a variety of applications, including use in conjunction with total ozone maps to create a daily tropospheric ozone product, as input to forecast models, or as a tool for validating independent ozone measurements when correlative data are not available. This technique is limited to regions where the ozone is a long-term tracer and the flow is adiabatic. We evaluate the internal consistency of the technique by transforming the ozone back to physical space and comparing to the original profiles. Biases in the long-term average of the differences are used to identify regions where the technique is consistently introducing errors. Initial results show the technique is useful in the lower stratosphere at most latitudes throughout the year,and in the winter hemisphere in the middle stratosphere. The results are problematic in the summer hemisphere middle stratosphere due to increased ozone photochemistry and weak PV gradients. Alternate techniques in these regions will be discussed. An additional limitation is the quality and resolution of the meteorological data.
Hollandsworth, Stacey M.↗