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NASA NTRS1976

Measurements of air pollutants over a Los Angeles freeway with a bistatic laser system

Nitric oxide, ozone, and ethylene were monitored over roads during periods of heavy traffic by transmitting several known laser wavelengths over an atmospheric path and measuring the differential absorption of the wavelengths. Heavy afternoon traffic between four and five o'clock over a 3.75 km path produced a noticeable increase in ethylene and a decrease in ozone. The changes occurred on a short time scale and correlated with the sudden traffic density increase. The ozone decrease occurs because of the sudden presence of large quantities of nitric oxide. Although the laboratory laser equipment used is rather cumbersome, the measurements did point out the potential of the laser absorption technique for monitoring large areas from one location.-

Menzies, R. T.↗

NASA NTRS1972

Possibilities of observing air pollution from orbital altitudes

Research carried out over a number of years has indicated the feasibility of monitoring global air pollution from orbiting satellites. Optical methods show considerable promise of measuring the burdens of pollution, both gaseous and particulates. Important pollution gases, such as sulfur dioxide, nitrogen dioxide, carbon monoxide, and ozone, as well as some hydrocarbon vapors, appear amenable to optical remote sensing. Satellite platforms for carrying out this work would not compete with ground monitoring stations but rather supplement them with a different type of data which could be integrated with ground level measurements to provide an all-embracing picture of pollution buildup, mass migration, and dissipation.

Barringer, A.↗

DOE OSTI2025

Detecting tropospheric composition and climate responses to US air pollution controls in the context of internally-arising variability

Since the 1970s, air pollutant emissions controls in the United States (US) have lowered concentrations of ozone (O 3 ) and aerosols, which have opposing radiative effects on surface temperature. Using a pair of initial-condition ensembles generated by a fully-coupled chemistry-climate model, we simulate the “world avoided” by US air pollution controls. In this counterfactual world, we find tropospheric column O 3 increases, robust to natural internal variability, extending across the Northern Hemisphere. Robust aerosol increases, dominated by sulfate, remain localized near the US. Wintertime Northwest Atlantic cloud droplet number concentration is particularly sensitive to US aerosol. While an ensemble mean US surface cooling signal (−0.4 °C) implies that aerosol-driven cooling prevails over any O 3 -induced warming, we find that large regional internal variability will confound its detection in any single transient realization. Larger signal-to-noise ratios for composition versus climate variables underscore the greater detectability of emissions-driven changes in tropospheric composition compared to their associated climate impacts.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1999

Biomass Burning Influences on the Composition of the Remote South Pacific Troposphere: Analysis Based on Observations from PEM Tropics-A

Airborne, in-situ measurements from PEM-Tropics-A (September/October 1996) are analyzed to show the presence of distinct pollution plumes in the middle-tropical troposphere of the remote South Pacific (10-30degS). These elevated plumes cause a relative maximum at about 5-7km attitude in the vertical distribution of primary and secondary species characteristic of fuel combustion and biomass burning (CO, C2H2, C2H6, CH3Cl, PAN, O3). Similar plumes were also observed at mid-latitudes in the middle troposphere during three flights east of New Zealand (40-45degS). In all, pollution plumes with CO larger than 100 ppb were observed 24 times on 7 separate flight days south of the equator. The observed plumes were generally embedded in very dry air. Ten-day back trajectory analysis supports the view that these originated from the biomass burning regions of South Africa (and South America) and were transported to the South Pacific along long-distance subsiding trajectories. The chemical composition of the southern Pacific troposphere analyzed from the PEM-Tropics-A data is compared with data from the tropical regions of the northern Pacific (PEM-West-A) and southern Atlantic (TRACE-A) during the same Sept/Oct time period. Sizable perturbations in the abundance of ozone and its key precursors, resulting from the transport of pollution originating from biomass burning sources, are observed in much of the Southern Hemispheric troposphere.

Singh, H. B.↗

NASA NTRS1994

Qualitative study of the behavior of minor species during a stratospheric warming with a 3-D model

It is well-known that the behavior of the ozone layer depends upon the coupling between several processes in the atmosphere. Natural or anthropogenic pollutants emitted from the surface or injected directly at high altitude may affect this layer. Assessment studies for long-term changes of the ozone layer are conducted with the aid of various two-dimensional models. These models describe the long-term and seasonal evolution of minor constituents and take into account the interaction between all processes. However, many limitations affect the self-consistency of these models e.g., the circulation in these models is only meridional and vertical and is not able to represent all types of motion in the atmosphere. During a perturbed winter in the north polar regions, the vortex is displaced from the pole to lower latitude so that wind may be reversed at a given location. Perturbed air masses are transported outside the darkened regions and may mix with local air masses. Three-dimensional models are the only tools which can describe correctly these sporadic phenomena.

Ramaroson, R.↗

NASA NTRS2001

SHADOZ (Southern Hemisphere ADditional Ozonesondes): A Look at the First Three Years' (1998-2000) Tropospheric Ozone Data

The first climatological overview of total, stratospheric and tropospheric ozone in the southern hemisphere tropical and subtropics is based on ozone sounding data from 10 sites comprising the Southern Hemisphere ADditional OZonesondes (SHADOZ) network. The period covered is 1998-2000. Observations were made over: Ascension Island; Nairobi, Kenya; Irene, South Africa; RCunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natai, Brazil. Campaign data were collected on a trans-Atlantic oceanographic cruise and during SAFARI-2000 in Zambia. The ozone data, with simultaneous temperature profiles to approx. 7 hPa and relative humidity to approx. 200 hPa, reside at an open archive: . SHADOZ ozone time-series and profiles give a perspective on tropical total, stratospheric and tropospheric ozone in 1998-2000. Prominent features are highly variable tropospheric ozone, a zonal wave-one pattern in total (and tropospheric) column ozone, and signatures of the Quasi-Biennial Oscillation (QBO) in stratospheric ozone. Total, stratospheric and tropospheric column ozone amounts peak between August and November and are lowest between March and May. Tropospheric ozone variability over the Indian and Pacific Ocean displays influences of the Indian Ocean Dipole, ENSO, and Madden-Julian circulation on convective mixing. Pollution transport from Africa, South American and the Maritime Continent is a seasonal feature. Tropospheric ozone seasonality over the Atlantic Basin shows effects of regional subsidence and recirculation as well as biomass burning. Dynamical and chemical influences appear to be of comparable magnitude.

Thompson, Anne M.↗

NASA NTRS2008

Quantifying VOC-Reaction Tracers, Ozone Production, and Continuing Aerosol Production Rates in Urban and Far-Downwind Atmospheres

We have found a surprisingly informative decomposition of the complex question of smoggy ozone production (basically, [HO2] in a more locally determined field of [NO]) in the process of linked investigations of modestly smoggy Eastern North America (by NASA aircraft, July 2004) and rather polluted Flushing, NYC (Queens College, July, 2001). In both rural and very polluted situations, we find that a simple contour graph parameterization of the local principal ozone production rate can be estimated using only the variables [NO] and j(sub rads) [HCHO]: Po(O3) = c (j(sub rads) [HCHO])(sup a) [HCHO](sup b). Here j(sub rads) is the photolysis of HCHO to radicals, presumably capturing many harder-UV photolytic processes and the principle ozone production is that due to HO2; mechanisms suggest that ozone production due to RO2 is closely correlated, often suggesting a limited range of different proportionality factors. The method immediately suggests a local interpretation for concepts of VOC limitation and NOx limitation. We believe that the product j(sub rads) [HCHO] guages the oxidation rate of observed VOC mixtures in a way that also provides [HO2] useful for the principle ozone production rate k [HO2] [NO], and indeed, all ozone chemical production. The success of the method suggests that dominant urban primary-HCHO sources may transition to secondary plume-HCHO sources in a convenient way. Are there other, simple, near-terminal oxidized VOC's which help guage ozone production and aerosol particle formation? Regarding particles, we report on, to the extent NASA Research resources allow, on appealing relationships between far-downwind (Atlantic PBL) HCHO and very fine aerosol (including sulfate. Since j(sub rads) [HCHO] provides a time-scale, we may understand distant-plume particle production in a more quantitative manner. Additionally we report on a statistical search in the nearer field for relationships between glyoxals (important near-terminal aromatic and isoprene reaction products) and aerosol production, looking for VOC's that might be most implicated. All three variables j(sub rads), [HCHO], and [NO] are relatively easily measured in widespread air pollution monitoring networks, and all are deducible form space-borne observations, though estimation of [NO] from [NO2] (the species observable from space) may require care. We report also on airborne and surface observations of HCHO, suggesting that concentrated (urban) and more diffuse (forest) sources may be distinguishable from space. The use of the 3.58 micron microwindow for HCHO remote sensing should allow much sharper resolution of HCHO than the UV. UV sensing requires large and expensive instruments, but even these seem justified since formaldehyde is so informative.

Chatfield, Robert↗

DOE OSTI2023

Comparing the Effect of Anthropogenically Amplified Halogen Natural Emissions on Tropospheric Ozone Chemistry Between Pre-Industrial and Present-Day

Reactive halogens (X + XO, X = I, Br or Cl) catalytically destroy a fraction of tropospheric ozone under present-day (PD) conditions, however, their distribution and potential impact on tropospheric ozone under pre-industrial (PI) conditions remain largely unexplored. This study uses the Community Atmosphere Model with Chemistry (CAM-Chem) to investigate the effect of anthropogenically amplified natural emissions of halogenated species and their subsequent chemistry on tropospheric ozone under PI and PD atmospheric conditions. Model results show that the global tropospheric ozone depletion due to natural halogens is slightly more sensitive in PI than PD, with percentage changes in tropospheric ozone burden (TOB) of -14.1 ± 0.6% for PI and -12.9 ± 0.6% for PD. Individually, the role of iodine and chlorine in ozone depletion is equivalent in both periods (ΔTOB I : ~-7% and ΔTOB Cl : ~-2.5%), while bromine plays a larger role in PI (ΔTOB Br : -5.5 ± 0.6%) versus PD (ΔTOB Br : -4.3 ± 0.7%). The increase in anthropogenic ozone precursor emissions from PI to PD has amplified the natural emission of inorganic halogens and led to a shift in the partitioning of inorganic halogens from reactive to reservoir species. Consequently, halogen-driven ozone depletion from the surface to the free troposphere is larger in PI than PD. In contrast, in the upper troposphere, the ozone depletion is larger in PD influenced mainly by stratospheric intrusion of reactive halogens from long-lived species. This study highlights the importance of including a complete chemical coupling of natural halogens and atmospheric pollutants in chemistry-climate models to adequately assess their effects on tropospheric ozone in a changing climate.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1988

Ozone measurements in the troposphere of an Amazonian rain forest environment

Ozone concentration profiles from the ground to above the stratospheric peak were obtained in an equatorial rain forest environment near Manaus in the Amazon Basin between July and August of 1985. The peak ozone concentration (4.4 x 10 to the 22 molecules/cu cm) was found at 20 mbar (26.6 km). A major pollution (biomass-burning) event which occurred near the end of the experiment was responsible for large changes in ozone concentration.

Kirchhoff, V. W. J. H.↗

NASA NTRS2014

Global Distribution and Trends of Tropospheric Ozone: An Observation-Based Review

Tropospheric ozone plays a major role in Earth's atmospheric chemistry processes and also acts as an air pollutant and greenhouse gas. Due to its short lifetime, and dependence on sunlight and precursor emissions from natural and anthropogenic sources, tropospheric ozone's abundance is highly variable in space and time on seasonal, interannual and decadal time-scales. Recent, and sometimes rapid, changes in observed ozone mixing ratios and ozone precursor emissions inspired us to produce this up-to-date overview of tropospheric ozone's global distribution and trends. Much of the text is a synthesis of in situ and remotely sensed ozone observations reported in the peer-reviewed literature, but we also include some new and extended analyses using well-known and referenced datasets to draw connections between ozone trends and distributions in different regions of the world. In addition, we provide a brief evaluation of the accuracy of rural or remote surface ozone trends calculated by three state-of-the-science chemistry-climate models, the tools used by scientists to fill the gaps in our knowledge of global tropospheric ozone distribution and trends.

Mixing ratios↗

NASA NTRS2002

Sources of Tropospheric Ozone along the Asian Pacific Rim: An Analysis of Ozonesonde Observations

The sources contributing to tropospheric ozone over the Asian Pacific Rim in different seasons are quantified by analysis of Hong Kong and Japanese ozonesonde observations with a global three-dimensional (3-D) chemical transport model (GEOS-CHEM) driven by assimilated meteorological observations. Particular focus is placed on the extensive observations available from Hong Kong in 1996. In the middle-upper troposphere (MT- UT), maximum Asian pollution influence along the Pacific Rim occurs in summer, reflecting rapid convective transport of surface pollution. In the lower troposphere (LT) the season of maximum Asian pollution influence shifts to summer at midlatitudes from fall at low latitudes due to monsoonal influence. The UT ozone minimum and high variability observed over Hong Kong in winter reflects frequent tropical intrusions alternating with stratospheric intrusions. Asian biomass burning makes a major contribution to ozone at less than 32 deg.N in spring. Maximum European pollution influence (less than 5 ppbv) occurs in spring in the LT. North American pollution influence exceeds European influence in the UT-MT, reflecting the uplift from convection and the warm conveyor belts over the eastern seaboard of North America. African outflow makes a major contribution to ozone in the low-latitude MT-UT over the Pacific Rim during November- April. Lightning influence over the Pacific Rim is minimum in summer due to westward UT transport at low latitudes associated with the Tibetan anticyclone. The Asian outflow flux of ozone to the Pacific is maximum in spring and fall and includes a major contribution from Asian anthropogenic sources year-round.

Liu, Hong-Yu↗

NASA NTRS2023

A Single-Point Modeling Approach for the Intercomparison and Evaluation of Ozone Dry Deposition Across Chemical Transport Models (Activity 2 of AQMEII4)

A primary sink of air pollutants and their precursors is dry deposition. Dry deposition estimates differ across chemical transport models, yet an understanding of the model spread is incomplete. Here, we introduce Activity 2 of the Air Quality Model Evaluation International Initiative Phase 4 (AQMEII4). We examine 18 dry deposition schemes from regional and global chemical transport models as well as standalone models used for impact assessments or process understanding. We configure the schemes as single-point models at eight Northern Hemisphere locations with observed ozone fluxes. Single-point models are driven by a common set of site-specific meteorological and environmental conditions. Five of eight sites have at least 3 years and up to 12 years of ozone fluxes. The interquartile range across models in multiyear mean ozone deposition velocities ranges from a factor of 1.2 to 1.9 annually across sites and tends to be highest during winter compared with summer. No model is within 50 % of observed multiyear averages across all sites and seasons, but some models perform well for some sites and seasons. For the first time, we demonstrate how contributions from depositional pathways vary across models. Models can disagree with respect to relative contributions from the pathways, even when they predict similar deposition velocities, or agree with respect to the relative contributions but predict different deposition velocities. Both stomatal and nonstomatal uptake contribute to the large model spread across sites. Our findings are the beginning of results from AQMEII4 Activity 2, which brings scientists who model air quality and dry deposition together with scientists who measure ozone fluxes to evaluate and improve dry deposition schemes in the chemical transport models used for research, planning, and regulatory purposes.

Dry deposition↗

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↗

DOE OSTI2023

A single-point modeling approach for the intercomparison and evaluation of ozone dry deposition across chemical transport models (Activity 2 of AQMEII4)

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1984

Airborne lidar observations of long-range transport in the free troposphere

Airborne lidar measurements of ozone and aerosols in the lower troposphere show the presence of pollutant layers above the mixed layer. Two case studies are analyzed to identify probable source regions and mechanisms for material injection into the free troposphere above local mixed layers. An elevated haze/oxidant layer observed over South Carolina on Aug. 2, 1980, was found to originate in cumulus convection over Georgia on Aug. 1, 1980. An extensive haze/oxidant layer observed over southeastern Virginia on July 31, 1981, is shown to have been in contact with the New England mixed layer on July 30, 1981. This transported air mass is estimated to contribute approximately 30 percent of the ozone maximum measured at the surface in the Norfolk, VA, area on July 31, 1981. Such elevated 'reservoir' layers are transported over long ranges and are not detected by sensors which are confined to the surface.

Shipley, S. T.↗

NASA NTRS2007

Reactive Nitrogen Distribution and Partitioning in the North American Troposphere and Lowermost Stratosphere

A comprehensive group of reactive nitrogen species (NO, NOz, HN03, HOzN02, PANs, alkyl nitrates, and aerosol-NO3) were measured over North America during July/August 2004 from the NASA DC-8 platform (0.1 - 12 km). Nitrogen containing tracers of biomass combustion (HCN and CH3CN) were also measured along with a host of other gaseous (CO, VOC, OVOC, halocarbon) and aerosol tracers. Clean background air as well as air with influences from biogenic emissions, anthropogenic pollution, biomass combustion, convection, lightning, and the stratosphere was sampled over the continental United States, the Atlantic, and the Pacific. The North American upper troposphere (UT) was found to be greatly influenced by both lightning NO, and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO,. Observational data suggest that lightning was a far greater contributor to NO, in the UT than previously believed. PAN provided a dominant reservoir of reactive nitrogen in the UT while nitric acid dominated in the lower troposphere (LT). Peroxynitric acid (H02N02) was present in sizable concentrations peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the LT. Plumes from Alaskan fires contained large amounts of PAN and aerosol nitrate but little enhancement in ozone. A comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. We investigate the partitioning and interplay of the reactive nitrogen species within characteristic air masses and further examine their role in ozone formation.

Singh, H. B.↗

NASA NTRS2008

The Aura Mission

Aura was designed to probe the chemistry of the troposphere as well as the stratosphere. Two instruments, the Microwave Limb Sounder, the Tropospheric Emission Spectrometer (TES) and the Ozone Monitoring Instrument (OMI) have provided some remarkable information on pollution, long range pollution transport and strat-trop exchange. This talk will review some of the more startling observations and some new science that we are seeing in the Aura data.

Schoeberl, Mark R.↗

NASA NTRS2012

Detecting Methane From Leaking Pipelines and as Greenhouse Gas in the Atmosphere

Laser remote sensing measurements of trace gases from orbit can provide unprecedented information about important planetary science and answer critical questions about planetary atmospheres. Methane (CH4) is the second most important anthropogenically produced greenhouse gas. Though its atmospheric abundance is much less than that of CO2 (1.78 ppm vs. 380 ppm), it has much larger greenhouse heating potential. CH4 also contributes to pollution in the lower atmosphere through chemical reactions, leading to ozone production. Atmospheric CH4 concentrations have been increasing as a result of increased fossil fuel production, rice farming, livestock, and landfills. Natural sources of CH4 include wetlands, wild fires, and termites, and perhaps other unknown sources. Important sinks for CH4 include non-saturated soils and oxidation by hydroxyl radicals in the atmosphere. Remotely measuring CH4 and other biogenic molecules (such as ethane and formaldehyde) on Mars also has important implications on the existence of life on Mars. Measuring CH4 at very low (ppb) concentrations from orbit will dramatically improve the sensitivity and spatial resolution in the search for CH4 vents and sub-surface life on other planets. A capability has been developed using lasers and spectroscopic detection techniques for the remote measurements of trace gases in open paths. Detection of CH4, CO2, H2O, and CO in absorption cells and in open paths, both in the mid- IR and near-IR region, has been demonstrated using an Optical Parametric Amplifier laser transmitter developed at GSFC. With this transmitter, it would be possible to develop a remote sensing methane instrument. CH4 detection also has very important commercial applications. Pipeline leak detection from an aircraft or a helicopter can significantly reduce cost, response time, and pinpoint the location. The main advantage is the ability to rapidly detect CH4 leaks remotely. This is extremely important for the petrochemical industry. This capability can be used in manned or unmanned airborne platforms for the detection of leaks in pipelines and other areas of interest where a CH4 leak is suspected.

Riris, Haris↗