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NASA NTRS1993

Effect of marine stratocumulus in TOMS ozone

The algorithm used to correct total O3 from the total ozone mapping spectrometer (TOMS) for cloud effects is based on the measured reflectivity, a climatological cloud top height, and an assumed tropospheric O3 column amount below clouds. In regions of persistent subtropical marine stratocumulus it is assumed that this introduces a positive error into total O3 because these clouds are lower than the assumed mean cloud height used in the algorithm. This appears to be confirmed by high correlation between Nimbus 7 TOMS total O3 and reflectivity data for typical regimes of persistent stratus, as identified by the international satellite cloud climatology project (ISCCP) observations. The TOMS total O3 overestimate has been computed using Nimbus 7/solar backscattered ultraviolet total O3 derived using temperature humidity infrared radiometer (THIR) data for years 1979-1984. A functional relationship between the THIR/non-THIR total O3 difference and reflectivity is used with TOMS reflectivity to modify Nimbus 7 TOMS O3 data for selected regions and periods. The correction diminishes or eliminates a number of apparent O3 maxima, with reductions of up to 20 Dobson units (DU) in total O3 on daily maps and approximately 5 DU on monthly mean O3 maps. Significant correlation between corrected TOMS O3 and reflectivity data remains because low-altitude O3 is retrieved more efficiently over a high-albedo surface. It is also possible that dynamical influences leading to stratocumulus formation bring O3-enriched air into the area. These results imply that although good arguments can be made for the use of TOMS total O3 as a proxy for tropospheric O3 in the tropics, caution must be exercised in the use of daily and even monthly O3 maps in the vicinity of clouds. Further research into the TOMS algorithm in cloudy regions is required to derive reliable estimates of tropospheric O3.

Thompson, A. M.↗

NASA NTRS2016

What is Eating Ozone? Thermal Reactions between SO2 And O3: Implications for Icy Environments

Laboratory studies are presented, showing for the first time that thermally driven reactions in solid H2O+SO2+O3 mixtures can occur below 150 K, with the main sulfur-containing product being bisulfate (HSO4(-)). Using a technique not previously applied to the low-temperature kinetics of either interstellar or solar system ice analogs, we estimate an activation energy of 32 kJ per mol for HSO4(-) formation. These results show that at the temperatures of the Jovian satellites, SO2 and O3 will efficiently react making detection of these molecules in the same vicinity unlikely. Our results also explain why O3 has not been detected on Callisto and why the SO2 concentration on Callisto appears to be highest on that world's leading hemisphere. Furthermore, our results predict that the SO2 concentration on Ganymede will be lowest in the trailing hemisphere, where the concentration of O3 is the highest. Our work suggests that thermal reactions in ices play a much more important role in surface and sub-surface chemistry than generally appreciated, possibly explaining the low abundance of sulfur-containing molecules and the lack of ozone observed in comets and interstellar ices.

Loeffler, Mark J.↗

NASA NTRS1990

Convection links biomass burning to increased tropical ozone - However, models will tend to overpredict O3

Biomass burning throughout the inhabited portions of the tropics generates precursors which lead to significant local atmospheric ozone pollution. Several simulations show how this smog could be only an easily observed, local manifestation of a much broader increase in tropospheric ozone. The basic processes are illustrated with a one-dimensional time-dependent model that is closer to true meteorological motions than commonly used eddy diffusion models. Its application to a representative region of South America gives reasonable simulations of the local pollutants measured there. Three illustrative simulations indicate the importance of dilution, principally due to vertical transport, in increasing the efficiency of ozone production, possibly enough for high ozone to be apparent on a very large, intercontinental scale.

Chatfield, Robert B.↗

NASA NTRS2015

Evaluating a New Homogeneous Total Ozone Climate Data Record from GOME/ERS-2, SCIAMACHY/Envisat, and GOME-2/MetOp-A

The European Space Agency's Ozone Climate Change Initiative (O3-CCI) project aims at producing and validating a number of high-quality ozone data products generated from different satellite sensors. For total ozone, the O3-CCI approach consists of minimizing sources of bias and systematic uncertainties by applying a common retrieval algorithm to all level 1 data sets, in order to enhance the consistency between the level 2 data sets from individual sensors. Here we present the evaluation of the total ozone products from the European sensors Global Ozone Monitoring Experiment (GOME)/ERS-2, SCIAMACHY/Envisat, and GOME-2/MetOp-A produced with the GOME-type Direct FITting (GODFIT) algorithm v3. Measurements from the three sensors span more than 16 years, from 1996 to 2012. In this work, we present the latest O3-CCI total ozone validation results using as reference ground-based measurements from Brewer and Dobson spectrophotometers archived at the World Ozone and UV Data Centre of the World Meteorological Organization as well as from UV-visible differential optical absorption spectroscopy (DOAS)/Système D′Analyse par Observations Zénithales (SAOZ) instruments from the Network for the Detection of Atmospheric Composition Change. In particular, we investigate possible dependencies in these new GODFIT v3 total ozone data sets with respect to latitude, season, solar zenith angle, and different cloud parameters, using the most adequate type of ground-based instrument. We show that these three O3-CCI total ozone data products behave very similarly and are less sensitive to instrumental degradation, mainly as a result of the new reflectance soft-calibration scheme. The mean bias to the ground-based observations is found to be within the 1 plus or minus 1 percent level for all three sensors while the near-zero decadal stability of the total ozone columns (TOCs) provided by the three European instruments falls well within the 1-3 percent requirement of the European Space Agency's Ozone Climate Change Initiative project.

Satellite sensors↗

NASA NTRS2006

SAGE III solar ozone measurements: Initial results

Results from two retrieval algorithms, o3-aer and o3-mlr , used for SAGE III solar occultation ozone measurements in the stratosphere and upper troposphere are compared. The main differences between these two retrieved (version 3.0) ozone are found at altitudes above 40 km and below 15 km. Compared to correlative measurements, the SAGE II type ozone retrievals (o3-aer) provide better precisions above 40 km and do not induce artificial hemispheric differences in upper stratospheric ozone. The multiple linear regression technique (o3_mlr), however, can yield slightly more accurate ozone (by a few percent) in the lower stratosphere and upper troposphere. By using SAGE III (version 3.0) ozone from both algorithms and in their preferred regions, the agreement between SAGE III and correlative measurements is shown to be approx.5% down to 17 km. Below 17 km SAGE III ozone values are systematically higher, by 10% at 13 km, and a small hemispheric difference (a few percent) appears. Compared to SAGE III and HALOE, SAGE II ozone has the best accuracy in the lowest few kilometers of the stratosphere. Estimated precision in SAGE III ozone is about 5% or better between 20 and 40 km and approx.10% at 50 km. The precision below 20 km is difficult to evaluate because of limited coincidences between SAGE III and sondes. SAGE III ozone values are systematically slightly larger (2-3%) than those from SAGE II but the profile shapes are remarkably similar for altitudes above 15 km. There is no evidence of any relative drift or time dependent differences between these two instruments for altitudes above 15-20 km.

Wang, Hsiang-Jui↗

NASA NTRSDate not supplied

Observations of So2, O3, and Aerosols With the Langley Mobile Ozone Lidar

LMOL, the NASA Langley Mobile Ozone Lidar, is located near NASA's LaRC steam plant when not deployed in campaigns. The steam plant is an incinerator, and when SO2 was in the plume, it would affect the LMOL O3 measurements at the plume altitudes of 100m-200m. In 2022, we modified LMOL to observe four wavelengths simultaneously to distinguish between and measure both O3 and SO2. With an optimized selection of wavelengths, based on an analysis of the cross-sections, it is possible to retrieve both O3 and SO2 densities from three wavelengths. Adding a fourth wavelength enables better constrains the aerosol's backscatter and extinction. In this work, we present the dual observations of SO2 and O3 with the new channels of LMOL, and we present the advances in constraining the aerosol parameters from these multiple wavelengths. We highlight the SO2 and Ozone Water-Land Environmental Transition Study (SOWLETS) campaign in preparation for the validation of the new system.

Guillaume Gronoff↗

NASA NTRS2002

Ozone Correction for AM0 Calibrated Solar Cells for the Aircraft Method

The aircraft solar cell calibration method has provided cells calibrated to space conditions for 37 years. However, it is susceptible to systematic errors due to ozone concentrations in the stratosphere. The present correction procedure applies a 1 percent increase to the measured I(sub SC) values. High band-gap cells are more sensitive to ozone absorbed wavelengths (0.4 to 0.8 microns) so it becomes important to reassess the correction technique. This paper evaluates the ozone correction to be 1+O3xFo, where O3 is the total ozone along the optical path, and Fo is 29.8 x 10(exp -6)/du for a Silicon solar cell, 42.6 x 10(exp -6)/du for a GaAs cell and 57.2 x 10(exp -6)/du for an InGaP cell. These correction factors work best to correct data points obtained during the flight rather than as a correction to the final result.

Snyder, David B.↗

NASA NTRS2008

The Effect of Lightning NOx Production on Surface Ozone in the Continental United States

Lightning NO(x) emissions calculated using the US National Lightning Detection Network data were found to account for 30% of the total NO(x) emissions for July August 2004, a period chosen both for having higher lightning NO(x) production and high ozone levels, thus maximizing the likelihood that such emissions could impact peak ozone levels. Including such emissions led to modest, but sometimes significant increases in simulated surface ozone when using the Community Multi-scale Air Quality Model (CMAQ). Three model simulations were performed, two with the addition of lightning NO(x) emissions, and one without. Domain-wide daily maximum 8-h ozone changes due to lightning NO(x) were less than 2 ppbv in 71 % of the cases with a maximum of 10 ppbv; whereas the difference in 1-h ozone was less than 2 ppbv in 77% of the cases with a maximum of 6 ppbv. Daily maximum 1-h and 8-h ozone for grids containing O3 monitoring stations changed slightly, with more than 43% of the cases differing less than 2 ppbv. The greatest differences were 42 ppbv for both 1-h and 8-h O3 , though these tended to be on days of lower ozone. Lightning impacts on the season-wide maximum 1-h and 8-h averaged ozone decreased starting from the 1 st to 4th highest values (an average of 4th highest, 8-h values is used for attainment demonstration in the US). Background ozone values from the y-intercept of O3 versus NO(z) curve were 42.2 and 43.9 ppbv for simulations without and with lightning emissions, respectively. Results from both simulations with lightning NO(x) suggest that while North American lightning production of NO(x) can lead to significant local impacts on a few occasions, they will have a relatively small impact on typical maximum levels and determination of Policy Relevant Background levels.

Kaynak, B.↗

NASA NTRS1992

Does UV instrumentation effectively measure ozone abundance?

Measurements of O3 on Mars provide significant information about the chemistry and composition of the atmosphere, including long-term changes. The most extensive and accurate data were inferred from the Mariner 9 UV spectrometer experiment. Mars O3 shows strong seasonal and latitudinal variation, with column abundances ranging from 0.2 microns at equatorial latitudes to 60 microns over the northern winter polar latitudes (1 micron-atm is a column abundance of 2.689 x 10(exp 15) molecules cm(exp-2)). The Mariner 9 UV spectrometer scanned from 2100 to 3500 Angstroms in one of its two spectral channels every 3 seconds with a spectral resolution of 15 Angstroms and an effective field-of-view of approximately 300 km(exp 2). Measurements were made for almost half a Martian year, with winter and spring in the Northern Hemisphere and summer and fall in the Southern Hemisphere. The detectability limit of the spectrometer was approximately 3 microns of ozone. The UV spectrometer on Mariner 9 was incapable of penetrating the dust during dust storms; the single-scattering albedo and phase function of airborne dust and cloud ice are not known to the degree required to extract the small UV signal reflected up from near the surface. The reflectance spectroscopy technique would also have difficulty detecting the total column abundance of O3 in cases where large dust abundances exist together with the polar hood, especially at high latitudes where large solar zenith angles magnify those optical depths; yet these cases would contain the maximum O3, based on theoretical results. It is quite possible that the maximum O3 column abundance observed by Mariner 9 of 60 microns is common. In fact, larger quantities may exist in some of the colder areas with optically thick clouds and dust. As the Viking period often had more atmospheric dust loading than did that of Mariner 9, the reflectance spectroscopy technique may even have been incapable of detecting the entire O3 column abundance during much of the Mars year that Viking observed, particularly at high latitudes.

Lindner, Bernhard Lee↗

NASA NTRS1981

A model study of the diurnal variation of mesospheric O3

Diurnal variation of ozone between 50 to 80 km is studied for both oxygen-only and O-N-H-C atmospheres. The temporal variation of ozone density along the ray path as well as that due to the change in the local zenith angle are included in the model computations. The difference between cases with and without the temporal variation of ozone density, is examined. It is found that the inclusion of this variation reduces the ozone concentration at all altitudes. In addition, the greatest effect on the ozone concentration is during sunrise and sunset.

Wang, P. H.↗

NASA NTRS2007

Mechanisms for the Intraseasonal Variability of Tropospheric Ozone over the Indian Ocean during the Winter Monsoon

We synthesize daily sonde (vertical) information and daily satellite (horizontal) information to provide an empirical description of ozone origins over the northern Indian Ocean during the INDOEX (Indian Ocean Experiment) field campaign (February-March 1999). This area is shown to be a significant portion of the "high-ozone tropics". East-west O3 features and their flow are identified, and ozone origins are compared to other tropical regions, using water vapor as a second tracer. In the study period, multiple processes contribute to O3 column enhancements, their importance varying strongly by latitude: (1) Low-altitude O3 pollution over the northern Indian Ocean mainly originates from the Indian subcontinent and is traceable to high emission areas. Convective activity south of Sri Lanka helps direct ozone outflow from the northern Indian subcontinent. (2) Middle tropospheric O3 maxima over the northern Indian Ocean originate from various sources, often transitioning within a few hours. Convective venting of Asian pollutants can add 20-30 ppbv to the middle troposphere at 5degN-10degN, alternating with stratospheric influence. (3) A number of cases suggest that strong mixing-in of stratospheric air along the subtropical jet raised tropospheric O3 in early March by approx.40-50 ppbv, especially poleward of approx. 10degN. (4) Influences of lightning and large-scale biomass burning were not strong during this period, in contrast to the situation in Africa and the South Atlantic or locally in Southeast Asia. This work illustrates successes and limitations in approaches to synthesizing disparate information on trace-gas distributions taken from satellite retrieval products and ozonesondes.

Chatfield, R. b.↗

NASA NTRS2020

Revisiting the Effectiveness Of HCHO/NO2 Ratios for Inferring Ozone Sensitivity to Its Precursors Using High Resolution Airborne Remote Sensing Observations in A High Ozone Episode During the KORUS-AQ Campaign

The nonlinear chemical processes involved in ozone production (P(O3)) have necessitated using proxy indicators to convey information about the primary dependence of P(O3) on volatile organic compounds (VOCs) or nitrogen oxides (NOx). In particular, the ratio of remotely sensed columns of formaldehyde (HCHO) to nitrogen dioxide (NO2) has been widely used for studying O3 sensitivity. Previous studies found that the errors in retrievals and the incoherent relationship between the column and the near-surface concentrations are a barrier in applying the ratio in a robust way. In addition to these obstacles, we provide calculational-observational evidence, using an ensemble of 0-D photochemical box models constrained by DC-8 aircraft measurements on an ozone event during the Korea-United States Air Quality (KORUS-AQ) campaign over Seoul, to demonstrate the chemical feedback of NO2 on the formation of HCHO is a controlling factor for the transition line between NOx-sensitive and NOx-saturated regimes. A fixed value (~2.7) of the ratio of the chemical loss of NOx (LNOx) to the chemical loss of HO2+RO2 (LROx) perceptibly differentiates the regimes. Following this value, data points with a ratio of HCHO/NO2 less than 1 can be safely classified as NOx-saturated regime, whereas points with ratios between 1 and 4 fall into one or the other regime. We attribute this mainly to the HCHO-NO2 chemical relationship causing the transition line to occur at larger (smaller) HCHO/NO2 ratios in VOC-rich (VOC-poor) environments. We then redefine the transition line to LNOx/LROx~2.7 that accounts for the HCHO-NO2 chemical relationship leading to HCHO = 3.7 × (NO2 – 1.14 × 1016 molec.cm-2). Although the revised formula is locally calibrated (i.e., requires for readjustment for other regions), its mathematical format removes the need for having a wide range of thresholds used in HCHO/NO2 ratios that is a result of the chemical feedback. Therefore, to be able to properly take the chemical feedback into consideration, the use of HCHO = a × (NO2 – b) formula should be preferred to the ratio in future works. We then use the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument to study O3 sensitivity in Seoul. The unprecedented spatial (250 × 250 m2) and temporal (~every 2 h) resolutions of HCHO and NO2 observations form the sensor enhance our understanding of P(O3) in Seoul; rather than providing a crude label for the entire city, more in-depth variabilities in chemical regimes are observed that should be able to inform mitigation strategies correspondingly.

KORUS-AQ; formaldehyde; NOx; VOC; OMI; GeoTASO; oz↗

NASA NTRS1988

Ground-based measurements of O3, NO2, OClO, and BrO during the 1987 Antarctic ozone depletion event

Near-ultraviolet absorption spectroscopy in the wavelength range from 330 to 370 nm was used to measure O3, NO2, OClO, and BrO at McMurdo Station (78S) during 1987. Visible absorption measurements of O3, NO2, and OClO were also obtained using the wavelength range from about 403 to 453 nm. These data are described and compared to observations obtained in 1986. It is shown that comparisons of observations in the two wavelength ranges provide a sensitive measure of the altitude where the bulk of atmospheric absorption takes place.

Sanders, R. W.↗

NASA NTRS2014

Wildfire Emissions and Their Interaction with Urban and Rural Pollution: Data and Simulations

In recent years NASA has conducted a series of airborne campaigns (e. g. SEAC4RS*, ARCTAS, INTEX-A/B) over North America using an instrumented DC-8 aircraft equipped to measure a very large number of gaseous and aerosol constituents including several unique tracers. In these campaigns wild fires were extensively sampled near source as well as downwind after aging. The data provided detailed information on the composition and chemistry of fire emissions under a variety of atmospheric conditions as well as their interactions with rural and urban air pollution. Major fires studied including the California Rim fire in 2013 (SEAC4RS), the 2008 California wildfires (ARCTAS), and the Alaskan fires downwind over eastern US (INTEX-A). Although some fire plumes contained virtually no O3 enhancement, others showed significant ozone formation. Over Los Angeles, the highest O3 mixing ratios were observed in fire influenced urban air masses. Attempts to simulate these interactions using state of the art models were only minimally successful and indicated several shortcomings in simulating fire emission influences on urban smog formation. A variety of secondary oxidation products (e. g. O3, PAN, HCHO) were substantially underestimated. We will discuss the data collected in fire influenced air masses and their potential air quality implications.

FIre Emissions↗

NASA NTRS1991

Effect of chemical kinetics uncertainties on calculated constituents in a tropospheric photochemical model

Random photochemical reaction rates are employed in a 1D photochemical model to examine uncertainties in tropospheric concentrations and thereby determine critical kinetic processes and significant correlations. Monte Carlo computations are used to simulate different chemical environments and their related imprecisions. The most critical processes are the primary photodissociation of O3 (which initiates ozone destruction) and NO2 (which initiates ozone formation), and the OH/methane reaction is significant. Several correlations and anticorrelations between species are discussed, and the ozone/transient OH correlation is examined in detail. One important result of the modeling is that estimates of global OH are generally about 25 percent uncertain, limiting the precision of photochemical models. Techniques for reducing the imprecision are discussed which emphasize the use of species and radical species measurements.

Thompson, Anne M.↗

NASA NTRS1992

How well is Martian ozone inferred with reflectance spectroscopy?

The Mariner 9 UV spectrometer scanned from 2100 to 3500 Angstroms in one of its two spectral channels every 3 seconds with a spectral resolution of 15 Angstroms and an effective field-of-view of approximately 300 km(exp 2). The only gaseous absorption in the 2000 to 3000 Angstrom region was assumed to come from the Hartley band system of ozone, and therefore the amount of ozone was inferred by fitting this absorption feature with laboratory data of ozone absorption. Mars O3 as inferred from these spectra shows strong seasonal and latitudinal variation, with column abundances ranging from 0.2 microns at equatorial latitudes to 60 microns over the northern winter polar latitudes. The detectability limit of the spectrometer was approximately 3 microns. I use a radiative transfer model based on the discrete ordinate method to calculate synthetic radiance spectra. When typical amounts of dust and cloud are present, significant underestimation of O3 occurs. A factor of 3 times as much O3 is needed to generate the same spectrum for cloudy, dusty atmospheres as for a clear atmosphere. If the scattering properties of Martian clouds and dust were well known, then their appearance would not be a problem, as a model would be capable of retrieving the O3 abundance. However, these properties are not well known, which raises doubts about the effectiveness of the current UV spectroscopy technique used to measure O3. Spatial and temporal variability in temperature and water vapor have been claimed to account for the scatter of the data points. However, water vapor is a small source of odd hydrogen in the winter polar atmosphere, and may not account for most of the variability. Masking by clouds and dust may also account for some of the observed O3 variability, because the nature and opacity of the clouds and dust in the polar hood change dramatically in latitude and even on a day-to-day basis. As the maximum O3 abundance resides near the surface, spacecraft must be able to observe through the entire cloud and dust abundance in order to actually see the total O3 column abundance. If reflectance spectroscopy is used, as on Mariner 9, then the cloud and the airborne dust must be traversed twice; first by the incoming solar flux down to the surface, and then once again upon reflection from the surface out to the spacecraft.

Lindner, Bernhard Lee↗

NASA NTRS2012

Validation of MIPAS IMK-IAA Temperature, Water Vapor, and Ozone Profiles with MOHAVE-2009 Campaign Measurements

MIPAS observations of temperature, water vapor, and ozone in October 2009 as derived with the scientific level-2 processor run by Karlsruhe Institute of Technology (KIT), Institute for Meteorology and Climate Research (IMK) and CSIC, Instituto de Astrofısica de Andalucıa (IAA) and retrieved from version 4.67 level-1b data have been compared to co-located field campaign observations obtained during the MOHAVE-2009 campaign at the Table Mountain Facility near Pasadena, California in October 2009. The MIPAS measurements were validated regarding any potential biases of the profiles, and with respect to their precision estimates. The MOHAVE-2009 measurement campaign provided measurements of atmospheric profiles of temperature, water vapor/relative humidity, and ozone from the ground to the mesosphere by a suite of instruments including radiosondes, ozonesondes, frost point hygrometers, lidars, microwave radiometers and Fourier transform infrared (FTIR) spectrometers. For MIPAS temperatures (version V4O_T_204), no significant bias was detected in the middle stratosphere; between 22 km and the tropopause MIPAS temperatures were found to be biased low by up to 2 K, while below the tropopause, they were found to be too high by the same amount. These findings confirm earlier comparisons of MIPAS temperatures to ECMWF data which revealed similar differences. Above 12 km up to 45 km, MIPAS water vapor (version V4O_H2O_203) is well within 10% of the data of all correlative instruments. The well-known dry bias of MIPAS water vapor above 50 km due to neglect of non-LTE effects in the current retrievals has been confirmed. Some instruments indicate that MIPAS water vapor might be biased high by 20 to 40% around 10 km (or 5 km below the tropopause), but a consistent picture from all comparisons could not be derived. MIPAS ozone (version V4O_O3_202) has a high bias of up to +0.9 ppmv around 37 km which is due to a non-identified continuum like radiance contribution. No further significant biases have been detected. Cross-comparison to co-located observations of other satellite instruments (Aura/MLS, ACE-FTS, AIRS) is provided as well.

MIPAS validation↗

NASA NTRS2006

Temperature-Dependence of Air-Broadened Line Widths and Shifts in the nu3 Band of Ozone

The 9.6-micron bands of O3 are used by many remote-sensing experiments for retrievals of terrestrial atmospheric ozone concentration profiles. Line parameter errors can contribute significantly to the total errors in these retrievals, particularly for nadir-viewing. The McMath-Pierce Fourier transform spectrometer at the National Solar Observatory on Kitt Peak was used to record numerous high-resolution infrared absorption spectra of O3 broadened by various gases at temperatures between 160 and 300 K. Over 30 spectra were analyzed simultaneously using a multispectrum nonlinear least squares fitting technique to determine Lorentz air-broadening and pressure-induced shift coefficients along with their temperature dependences for selected transitions in the 3 fundamental band of (16)O3. We compare the present results with other measurements reported in the literature and with the ozone parameters on the 2000 and 2004 editions of the HITRAN database.

Smith, Mary A. H.↗