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NASA NTRS2017

Causes of Interannual Variability over the Southern Hemispheric Tropospheric Ozone Maximum

We examine the relative contribution of processes controlling the interannual variability (IAV) of tropospheric ozone over four sub-regions of the southern hemispheric tropospheric ozone maximum (SHTOM) over a 20-year period. Our study is based on hindcast simulations from the National Aeronautics and Space Administration Global Modeling Initiative chemistry transport model (NASA GMI-CTM) of tropospheric and stratospheric chemistry, driven by assimilated Modern Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Our analysis shows that over SHTOM region, the IAV of the stratospheric contribution is the most important factor driving the IAV of upper tropospheric ozone (270 hectopascals), where ozone has a strong radiative effect. Over the South Atlantic region, the contribution from surface emissions to the IAV of ozone exceeds that from stratospheric input at and below 430 hectopascals. Over the South Indian Ocean, the IAV of stratospheric ozone makes the largest contribution to the IAV of ozone with little or no influence from surface emissions at 270 and 430 hectopascals in austral winter. Over the tropical South Atlantic region, the contribution from IAV of stratospheric input dominates in austral winter at 270 hectopascals and drops to less than half but is still significant at 430 hectopascals. Emission contributions are not significant at these two levels. The IAV of lightning over this region also contributes to the IAV of ozone in September and December. Over the tropical southeastern Pacific, the contribution of the IAV of stratospheric input is significant at 270 and 430 hectopascals in austral winter, and emissions have little influence.

Global Modeling Initiative chemistry transport mod↗
NASA NTRS1987

The use of TOMS data for tropospheric ozone studies

Instances were identified where enhancements of tropical ozone are associated with sporadic widespread biomass burning. A strong positive correlation exists between total ozone and the distribution of carbon monoxide in the tropics, indicating that total ozone data can be used for tropospheric ozone studies. Using ozone profiles derived from the Stratospheric Aerosol and Gas Experiment (SAGE), preliminary findings show enhanced tropospheric ozone concentrations over Africa and the eastern Atlantic at tropical latitudes. Other preliminary studies also suggest that Total Ozone Mapping Spectrometer (TOMS) data may provide a means of identifying widespread air pollution episodes over the United States during the summer.

Fishman, Jack↗
NASA NTRS1979

Observational and theoretical evidence in support of a significant in-situ photochemical source of tropospheric ozone

The latitudinal and seasonal variation of ozone in the troposphere is discussed. Of particular interest is the asymmetrical behavior of this gas with respect to the two hemispheres. These asymmetries, when coupled with a diagnostic photochemical model of the troposphere, lends support to the view that ozone cannot be viewed as an inert tracer of stratospheric origin. In the calculations it is noted that it is likely that the budgets of carbon monoxide and tropospheric ozone may be quite dependent on each other and the calculations are discussed in light of the uncertainty which currently exists about representative global tropospheric background concentrations of the nitrogen oxides. In addition, the seasonal variation of excess (C-14)O2 (a stratospheric tracer) is examined and compared with the seasonal ozone variation during the same period of observations at the same location and altitudes. The distinct maxima for ozone found during the summer in the lower troposphere are not present for the (C-14)O2 data. This finding likewise suggests that photochemical processes taking place in the troposphere are an important source term for tropospheric ozone.

Fishman, J.↗
NASA NTRS2000

Satellite Observations of Enhanced Tropospheric Ozone Associated with Biomass Burning in Africa and Madagascar

Tropospheric ozone over Africa and Madagascar is enhanced by 10 to 15 DU in October. This maximum coincides with the time of maximum biomass area burning in Africa and Madagascar. Ozone observations were made from 1979 to 1999 using the TOMS tropospheric ozone convective cloud differential method. As a result of easterly trade winds, ozone originating on Madagascar is transported to the west over the Mozambique Channel. In El Nino years higher level westerly winds descend to transport low level ozone easterly. This results in African continental ozone being transported east of Madagascar. Long range transport of African ozone is observed during El Nino periods.

Aikin, A. C.↗
NASA NTRS2009

Recent Biomass Burning in the Tropics and Related Changes in Tropospheric Ozone

Biomass burning is an important source of chemical precursors of tropospheric ozone. In the tropics, biomass burning produces ozone enhancements over broad regions of Indonesia, Africa, and South America including Brazil. Fires are intentionally set in these regions during the dry season each year to clear cropland and to clear land for human/industrial expansion. In Indonesia enhanced burning occurs during dry El Nino conditions such as in 1997 and 2006. These burning activities cause enhancement in atmospheric particulates and trace gases which are harmful to human health. Measurements from the Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) from October 2004-November 2008 are used to evaluate the effects of biomass burning on tropical tropospheric ozone. These measurements show sizeable decreases approx.15-20% in ozone in Brazil during 2008 compared to 2007 which we attribute to the reduction in biomass burning. Three broad biomass burning regions in the tropics (South America including Brazil, western Africa, and Indonesia) were analyzed in the context of OMI/MLS measurements and the Global Modeling Initiative (GMI) chemical transport model developed at Goddard Space Flight Center. The results indicate that the impact of biomass burning on ozone is significant within and near the burning regions with increases of approx.10-25% in tropospheric column ozone relative to average background concentrations. The model suggests that about half of the increases in ozone from these burning events come from altitudes below 3 km. Globally the model indicates increases of approx.4-5% in ozone, approx.7-9% in NO, (NO+NO2), and approx.30-40% in CO.

Ziemke↗
NASA NTRS2016

Evaluating A Priori Ozone Profile Information Used in TEMPO Tropospheric Ozone Retrievals

Ozone (O3) is a greenhouse gas and toxic pollutant which plays a major role in air quality. Typically, monitoring of surface air quality and O3 mixing ratios is primarily conducted using in situ measurement networks. This is partially due to high-quality information related to air quality being limited from space-borne platforms due to coarse spatial resolution, limited temporal frequency, and minimal sensitivity to lower tropospheric and surface-level O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite is designed to address these limitations of current space-based platforms and to improve our ability to monitor North American air quality. TEMPO will provide hourly data of total column and vertical profiles of O3 with high spatial resolution to be used as a near-real-time air quality product. TEMPO O3 retrievals will apply the Smithsonian Astrophysical Observatory profile algorithm developed based on work from GOME, GOME-2, and OMI. This algorithm uses a priori O3 profile information from a climatological data-base developed from long-term ozone-sonde measurements (tropopause-based (TB) O3 climatology). It has been shown that satellite O3 retrievals are sensitive to a priori O3 profiles and covariance matrices. During this work we investigate the climatological data to be used in TEMPO algorithms (TB O3) and simulated data from the NASA GMAO Goddard Earth Observing System (GEOS-5) Forward Processing (FP) near-real-time (NRT) model products. These two data products will be evaluated with ground-based lidar data from the Tropospheric Ozone Lidar Network (TOLNet) at various locations of the US. This study evaluates the TB climatology, GEOS-5 climatology, and 3-hourly GEOS-5 data compared to lower tropospheric observations to demonstrate the accuracy of a priori information to potentially be used in TEMPO O3 algorithms. Here we present our initial analysis and the theoretical impact on TEMPO retrievals in the lower troposphere.

ozone↗
NASA NTRS2016

Understanding the Laminar Distribution of Tropospheric Ozone from Ground-Based, Airborne, Spaceborne, and Modeling Perspectives

Laminar ozone structure is a ubiquitous feature of tropospheric-ozone distributions resulting from dynamic and chemical atmospheric processes. Understanding the characteristics of these ozone laminae and the mechanisms responsible for producing them is important to outline the transport pathways of trace gases and to quantify the impact of different sources on tropospheric background ozone. In this study, we present a new method to detect ozone laminae to understand their climatological characteristics of occurrence frequency in terms of thickness and altitude. We employ both ground-based and airborne ozone lidar measurements and other synergistic observations and modeling to investigate the sources and mechanisms such as biomass burning transport, stratospheric intrusion, lightning-generated NOx, and nocturnal low-level jets that are responsible for depleted or enhanced tropospheric ozone layers. Spaceborne (e.g., OMI (Ozone Monitoring Instrument), TROPOMI (Tropospheric Monitoring Instrument), TEMPO (Tropospheric Emissions: Monitoring of Pollution)) measurements of these laminae will observe greater horizontal extent and lower vertical resolution than balloon-borne or lidar measurements will quantify. Using integrated ground-based, airborne, and spaceborne observations in a modeling framework affords insight into how to gain knowledge of both the vertical and horizontal evolution of these ubiquitous ozone laminae.

Tropospheric Ozone↗
NASA NTRS2006

Role of Climate Change in Global Predictions of Future Tropospheric Ozone and Aerosols

A unified tropospheric chemistry-aerosol model within the Goddard Institute for Space Studies general circulation model II is applied to simulate an equilibrium CO2-forced climate in the year 2100 to examine the effects of climate change on global distributions of tropospheric ozone and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols. The year 2100 CO2 concentration as well as the anthropogenic emissions of ozone precursors and aerosols/aerosol precursors are based on the Intergovernmental Panel on Climate Change Special Report on Emissions Scenarios (SRES) A2. Year 2100 global O3 and aerosol burdens predicted with changes in both climate and emissions are generally 5-20% lower than those simulated with changes in emissions alone; as exceptions, the nitrate burden is 38% lower, and the secondary organic aerosol burden is 17% higher. Although the CO2-driven climate change alone is predicted to reduce the global O3 concentrations over or near populated and biomass burning areas because of slower transport, enhanced biogenic hydrocarbon emissions, decomposition of peroxyacetyl nitrate at higher temperatures, and the increase of O3 production by increased water vapor at high NOx levels. The warmer climate influences aerosol burdens by increasing aerosol wet deposition, altering climate-sensitive emissions, and shifting aerosol thermodynamic equilibrium. Climate change affects the estimates of the year 2100 direct radiative forcing as a result of the climate-induced changes in burdens and different climatological conditions; with full gas-aerosol coupling and accounting for ozone and direct radiative forcings by the O2, sulfate, nitrate, black carbon, and organic carbon are predicted to be +0.93, -0.72, -1.0, +1.26, and -0.56 W m(exp -2), respectively, using present-day climate and year 2100 emissions, while they are predicted to be +0.76, -0.72, 0.74, +0.97, and -0.58 W m(exp -2), respectively, with year 2100 climate and emissions.

Liao, Hong↗
NASA NTRS1989

The global consequences of increasing tropospheric ozone concentrations

Recent analyses of long term records of tropospheric ozone measurements in the Northern Hemisphere suggest that it is increasing at a rate of 1 to 2 percent per year. Because of this, it is argued that the amount of atmospheric warming due to increasing tropospheric ozone is comparable to, or possibly even greater than, the amount of warming due to the increase of carbon dioxide. Unlike all other climatically important trace gases, ozone is toxic, and increases in its concentration will result in serious environmental damage, as well as impairment of human health.

Fishman, Jack↗
NASA NTRS2004

Feasibility of Sensing Tropospheric Ozone with MODIS 9.6 Micron Observations

With the infrared observations made by the Moderate Resolution Imaging Spectrometer (MODIS) on board the EOS-Aqua satellite, which include the 9.73 micron channel, a method is developed to deduce horizontal patterns of tropospheric ozone in cloud free conditions on a scale of about 100 km. It is assumed that on such small scale, at a given instant, horizontal changes in stratospheric ozone are small compared to that in the troposphere. From theoretical simulations it is found that uncertainties in the land surface emissivity and the vertical thermal stratification in the troposphere can lead to significant errors in the inferred tropospheric ozone. Because of this reason in order to derive horizontal patterns of tropospheric ozone in a given geographic area a tuning of this method is necessary with the help of a few dependent cases. After tuning, this method is applied to independent cases of MODIS data taken over Los Angeles basin in cloud free conditions to derive horizontal distribution of ozone in the troposphere. Preliminary results indicate that the derived patterns of ozone resemble crudely the patterns of surface ozone reported by EPA.

Prabhakara, C.↗
NASA NTRS2004

Tropical Tropospheric Ozone Climatology: Approaches Based on SHADOZ Observations

The SHADOZ (Southern Hemisphere Additional Ozonesondes) ozone sounding network was initiated in 1998 to improve the coverage of tropical in-situ ozone measurements for satellite validation, algorithm development and related process studies. Over 2000 soundings have been archived at the central website, , for 12 stations that span the entire equatorial zone [Thompson et al., JGR, 108,8238, 2003]. The most striking features of tropospheric ozone profiles in SHADOZ are: (1) persistent longitudinal variability in tropospheric ozone profiles, with a 10-15 DU column-integrated difference between Atlantic and Pacific sites; (2) intense short-term variability triggered by changing meteorological conditions and advection of pollution. The implications of these results for profile climatologies and trends are described along with several approaches to classifying ozone profiles: 1) Seasonal means during MAM (March-April-May) and SON (September-October-November); 2) Maxima and minima, identified through correlation of TOMS-derived TTO (tropical tropospheric ozone) column depth with the sonde integrated tropospheric ozone column; and 3) Meteorological regimes, a technique that is effective in the subtropics where tropical and mid-latitude conditions alternate.

Thompson, Anne M.↗
NASA NTRS1986

Use of satellite data to study tropospheric ozone in the tropics

Three independent examples are discussed which suggest that photochemical ozone production in the troposphere can be observed in the tropics from an analysis of total ozone data. The first finding shows that the seasonal cycle of total columnar ozone is dominated by the seasonal cycle of tropospheric ozone, even though tropospheric ozone accounts for only 5-15 percent of the total ozone. Second, a case study is presented which shows that enhanced total ozone observed over the Amazon Basin can be associated with the presence of biomass burning. In situ measurements have confirmed that biomass burning does result in the production of photochemically generated ozone, analogous to the formation of 'smog' near industrialized areas. Third, an analysis of the distribution of carbon monoxide obtained from a Space Shuttle platform is strongly correlated with the concurrent distribution of total ozone between 5 deg S and 10 deg N. Because all of the sources of carbon monoxide are located in the troposphere, this finding likewise suggests that the gradients of total ozone at low latitudes must also reflect processes occurring in the troposphere.

Fishman, Jack↗
NASA NTRS1979

Application of a microprocessor controlled lidar to tropospheric ozone measurements

A microprocessor controlled lidar system under construction at the NASA Goddard Space Flight Center is described and the problems in making space-based measurements of tropospheric ozone are considered. The differential absorption lidar using a dual wavelength, pulsed CO2 laser and direct detection receiver can significantly improve the existing global data base on tropospheric ozone burden. Sensitivity to tropospheric ozone can be obtained in the spaceborne version of lidar by selecting laser lines located in the wings of the target zone lines. Simulation studies using various laser line pairs in the P-branch of the CO2 9.4 micron band show that the ozone burden retrieval may be weighted to particular altitude regions. These simulation studies are based on numerical integration of differences in absorption coefficient at the two selected laser wavelengths using the AFGL absorption line parameter compilations, U.S. Standard Atmosphere ozone profile, and laser software. Simulation, data collection and reduction are performed by a microprocessor subsystem of the CO2 lidar.

Stewart, R. W.↗
NASA NTRS1991

The global consequences of increasing tropospheric ozone concentrations

Recent analyses of long-term records of tropospheric ozone measurements in the Northern Hemisphere suggest that it is increasing at a rate of 1 to 2 percent per year. Because of this, it is argued that the amount of atmospheric warming due to increasing tropospheric ozone is comparable to, or possibly even greater than, the amount of warming due to the increase of carbon dioxide. Unlike all other climatically important trace gases, ozone is toxic, and increases in its concentration will result in serious environmental damage, as well as impairment of human health.

Fishman, Jack↗
NASA NTRS1997

Remote Sensing of Tropospheric Ozone and Its Precursors

Global and regional mapping of tropospheric ozone and its precursors using the Tropospheric Emission Spectrometer and its forerunner - the Airborne Emission Spectrometer - will be discussed.

ozone troposphere spectrometry Tropospheric Emissi↗
NASA NTRS1991

Raman shifting of KrF laser radiation for tropospheric ozone measurements

The differential absorption lidar (DIAL) measurement of tropospheric ozone requires use of high average power UV lasers operating at two appropriate DIAL wavelengths. Laboratory experiments have demonstrated that a KrF excimer laser can be used to generate several wavelengths with good energy conversion efficiencies by stimulated Raman shifting using hydrogen (H2) and deuterium (D2). Computer simulations for an airborne lidar have shown that these laser emissions can be used for the less than 5 percent random error, high resolution measuremment of ozone across the troposphere using the DIAL technique. In the region of strong ozone absorption, laser wavelengths of 277.0 and 291.7 nm were generated using H2 and D2, respectively. In addition, a laser wavelength at 302.0 nm was generated using two cells in series, with the first containing D2 and the second containing H2. The energy conversion efficiency for each wavelength was between 14 and 27 percent.

Grant, William B.↗
NASA NTRS2017

Evaluating a Priori Ozone Profile Information Used in TEMPO (Tropospheric Emissions: Monitoring of Pollution) Tropospheric Ozone Retrievals

A primary objective for TOLNet is the evaluation and validation of space-based tropospheric O3 retrievals from future systems such as the Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite. This study is designed to evaluate the tropopause-based O3 climatology (TB-Clim) dataset which will be used as the a priori profile information in TEMPO O3 retrievals. This study also evaluates model simulated O3 profiles, which could potentially serve as a priori O3 profile information in TEMPO retrievals, from near-real-time (NRT) data assimilation model products (NASA Global Modeling and Assimilation Office (GMAO) Goddard Earth Observing System (GEOS-5) Forward Processing (FP) and Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA2)) and full chemical transport model (CTM), GEOS-Chem, simulations. The TB-Clim dataset and model products are evaluated with surface (0-2 km) and tropospheric (0-10 km) TOLNet observations to demonstrate the accuracy of the suggested a priori dataset and information which could potentially be used in TEMPO O3 algorithms. This study also presents the impact of individual a priori profile sources on the accuracy of theoretical TEMPO O3 retrievals in the troposphere and at the surface. Preliminary results indicate that while the TB-Clim climatological dataset can replicate seasonally-averaged tropospheric O3 profiles observed by TOLNet, model-simulated profiles from a full CTM (GEOS-Chem is used as a proxy for CTM O3 predictions) resulted in more accurate tropospheric and surface-level O3 retrievals from TEMPO when compared to hourly (diurnal cycle evaluation) and daily-averaged (daily variability evaluation) TOLNet observations. Furthermore, it was determined that when large daily-averaged surface O3 mixing ratios are observed (65 ppb), which are important for air quality purposes, TEMPO retrieval values at the surface display higher correlations and less bias when applying CTM a priori profile information compared to all other data products. The primary reason for this is that CTM predictions better capture the spatio-temporal variability of the vertical profiles of observed tropospheric O3 compared to the TB-Clim dataset and other NRT data assimilation models evaluated during this study.

Pollution↗
NASA NTRS2004

Interpretation of TOMS Observations of Tropical Tropospheric Ozone with a Global Model and In Situ Observations

We interpret the distribution of tropical tropospheric ozone columns (TTOCs) from the Total Ozone Mapping Spectrometer (TOMS) by using a global three-dimensional model of tropospheric chemistry (GEOS-CHEM) and additional information from in situ observations. The GEOS-CHEM TTOCs capture 44% of the variance of monthly mean TOMS TTOCs from the convective cloud differential method (CCD) with no global bias. Major discrepancies are found over northern Africa and south Asia where the TOMS TTOCs do not capture the seasonal enhancements from biomass burning found in the model and in aircraft observations. A characteristic feature of these northern topical enhancements, in contrast to southern tropical enhancements, is that they are driven by the lower troposphere where the sensitivity of TOMS is poor due to Rayleigh scattering. We develop an efficiency correction to the TOMS retrieval algorithm that accounts for the variability of ozone in the lower troposphere. This efficiency correction increases TTOC's over biomass burning regions by 3-5 Dobson units (DU) and decreases them by 2-5 DU over oceanic regions, improving the agreement between CCD TTOCs and in situ observations. Applying the correction to CCD TTOCs reduces by approximately DU the magnitude of the "tropical Atlantic paradox" [Thompson et al, 2000], i.e. the presence of a TTOC enhancement over the southern tropical Atlantic during the northern African biomass burning season in December-February. We reproduce the remainder of the paradox in the model and explain it by the combination of upper tropospheric ozone production from lightning NOx, peristent subsidence over the southern tropical Atlantic as part of the Walker circulation, and cross-equatorial transport of upper tropospheric ozone from northern midlatitudes in the African "westerly duct." These processes in the model can also account for the observed 13-17 DU persistent wave-1 pattern in TTOCs with a maximum above the tropical Atlantic and a minimum over the tropical Pacific during all seasons. The photochemical effects of mineral dust have only a minor role on the modeled distribution of TTOCs, including over northern Africa, due to multiple competing effects. The photochemical effects of mineral dust globally decease annual mean OH concentrations by 9%. A global lightning NOx source of 6 Tg N yr(sup -1) in the model produces a simulation that is most consistent with TOMS and in situ observations.

Martin, Randall V.↗