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Leveraging Scientific Community Knowledge for Air Quality Model Chemistry Parameterizations

Air pollution contributes to adverse health outcomes. Approximately 121 million people in the United States—one third of the population—live where National Ambient Air Quality Standards (NAAQS) are violated. In most cases, the criteria pollutants exceeding standards are ozone (O 3 ) and fine particles (PM 2.5 ). In addition, 188 substances known or suspected to cause cancer or other serious health effects are designated as hazardous air pollutants (HAPs). Essentially, all O 3 and significant portions of PM 2.5 and HAPs are produced in the atmosphere through chemical and physical processes. In the case of PM 2.5 , subcomponents formed primarily from precursor gases—sulfate, nitrate, ammonium, and secondary organic aerosol (SOA)—account for 60% of the U.S. county-level annual mean concentration. In addition, 47% of the cancer risk and 25% of the noncancer risk from HAPs have been attributed to atmospheric chemistry rather than direct emissions. In this article, we introduce the role of chemical mechanisms in air quality models, a new atmospheric science community effort, and needs for further mechanism development.

Havala O.T. Pye↗

Tropospheric Ozone Change from 1980 to 2010 Dominated by Equatorward Redistribution of Emissions

Ozone is an important air pollutant at the surface, and the third most important anthropogenic greenhouse gas in the troposphere. Since 1980, anthropogenic emissions of ozone precursors methane, non-methane volatile organic compounds, carbon monoxide and nitrogen oxides (NOx) have shifted from developed to developing regions. Emissions have thereby been redistributed equatorwards, where they are expected to have a stronger effect on the tropospheric ozone burden due to greater convection, reaction rates and NOx sensitivity. Here we use a global chemical transport model to simulate changes in tropospheric ozone concentrations from 1980 to 2010, and to separate the influences of changes in the spatial distribution of global anthropogenic emissions of short-lived pollutants, the magnitude of these emissions, and the global atmospheric methane concentration. We estimate that the increase in ozone burden due to the spatial distribution change slightly exceeds the combined influences of the increased emission magnitude and global methane. Emission increases in Southeast, East and South Asia may be most important for the ozone change, supported by an analysis of statistically significant increases in observed ozone above these regions. The spatial distribution of emissions dominates global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from low latitudes.

Zhang, Yuqiang↗

The Effect of Future Ambient Air Pollution on Human Premature Mortality to 2100 Using Output from the ACCMIP Model Ensemble

Ambient air pollution from ground-level ozone and fine particulate matter (PM(sub 2.5)) is associated with premature mortality. Future concentrations of these air pollutants will be driven by natural and anthropogenic emissions and by climate change. Using anthropogenic and biomass burning emissions projected in the four Representative Concentration Pathway scenarios (RCPs), the ACCMIP ensemble of chemistry climate models simulated future concentrations of ozone and PM(sub 2.5) at selected decades between 2000 and 2100. We use output from the ACCMIP ensemble, together with projections of future population and baseline mortality rates, to quantify the human premature mortality impacts of future ambient air pollution. Future air-pollution-related premature mortality in 2030, 2050 and 2100 is estimated for each scenario and for each model using a health impact function based on changes in concentrations of ozone and PM(sub 2.5) relative to 2000 and projected future population and baseline mortality rates. Additionally, the global mortality burden of ozone and PM(sub 2.5) in 2000 and each future period is estimated relative to 1850 concentrations, using present-day and future population and baseline mortality rates. The change in future ozone concentrations relative to 2000 is associated with excess global premature mortality in some scenarios/periods, particularly in RCP8.5 in 2100 (316 thousand deaths per year), likely driven by the large increase in methane emissions and by the net effect of climate change projected in this scenario, but it leads to considerable avoided premature mortality for the three other RCPs. However, the global mortality burden of ozone markedly increases from 382000 (121000 to 728000) deaths per year in 2000 to between 1.09 and 2.36 million deaths per year in 2100, across RCPs, mostly due to the effect of increases in population and baseline mortality rates. PM(sub 2.5) concentrations decrease relative to 2000 in all scenarios, due to projected reductions in emissions, and are associated with avoided premature mortality, particularly in 2100: between 2.39 and 1.31 million deaths per year for the four RCPs. The global mortality burden of PM(sub 2.5) is estimated to decrease from 1.70 (1.30 to 2.10) million deaths per year in 2000 to between 0.95 and 1.55 million deaths per year in 2100 for the four RCPs due to the combined effect of decreases in PM(sub 2.5) concentrations and changes in population and baseline mortality rates. Trends in future air-pollution-related mortality vary regionally across scenarios, reflecting assumptions for economic growth and air pollution control specific to each RCP and region. Mortality estimates differ among chemistry climate models due to differences in simulated pollutant concentrations, which is the greatest contributor to overall mortality uncertainty for most cases assessed here, supporting the use of model ensembles to characterize uncertainty. Increases in exposed population and baseline mortality rates of respiratory diseases magnify the impact on premature mortality of changes in future air pollutant concentrations and explain why the future global mortality burden of air pollution can exceed the current burden, even where air pollutant concentrations decrease.

Silva, Raquel A.↗

Recent Changes in Tropospheric Ozone in the Tropics

This paper presents a detailed characterization of tropical tropospheric column ozone variability on time scales varying from a few days to a solar cycle. The study is based on more than 20 years (1979 to the present) of tropospheric column ozone time series derived from the convective cloud differential (CCD) method using total ozone mapping spectrometer (TOMS) data. Results indicate three distinct regions in the tropics with distinctly three different zonal characteristics related to seasonal, interannual and solar variabilities. These three regions are the eastern Pacific, Atlantic, and western Pacific. Tropospheric column ozone in the Atlantic region peaks at about the same time (September-October) from 20 N to 20 S. The amplitude of the annual cycle, however, varies from about 3 to 6 Dobson unit (DU) from north to south of the equator. In comparison, the annual cycle in both the eastern and western Pacific is generally week and the phase varies from peak values in March and April in the northern hemisphere to September and October in the southern hemisphere. The interannual pattern in the three regions are also very different. The Atlantic region indicates a quasi biennial oscillation in the tropospheric column ozone which is out of phase with the stratospheric ozone. This is consistent with the photochemical control of this region caused by high pollution and high concentration of ozone producing precursors. The observed pattern, however, does not seem to be related to the interannual variability in ozone precursors related to biomass burning. Instead, it appears to be a manifestation of the UV modulation of upper tropospheric chemistry on a QBO time scale caused by stratospheric ozone. During El Nino events, there is anomalously low ozone in the eastern Pacific and high values in the western Pacific indicating the effects of convectively driven transport. The observed increase of 10-20 DU in tropospheric column ozone in the Indonesian region in the western Pacific during the recent 1997-1998 El Nino was associated with large-scale forest fires which may have contributed 5-10 DU of the total increase.

Chandra, S.↗

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

A comprehensive group of reactive nitrogen species (NO, NO2, HNO3, HO2NO2, PANs, alkyl nitrates, and aerosol-NO3) were measured in the troposphere and lowermost stratosphere over North America and the Atlantic during July/August 2004 (INTEX-A) from the NASA DC-8 platform (0.1-12 km). Less reactive nitrogen species (HCN and CH3CN), that are also unique tracers of biomass combustion, 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, and stratosphere was sampled both over continental U. S., Atlantic and Pacific. The North American upper troposphere was found to be greatly influenced by both lightning NO(x) and surface pollution lofted via convection and contained elevated concentrations of PAN, ozone, hydrocarbons, and NO(x). Under polluted conditions PAN was a dominant carrier of reactive nitrogen in the upper troposphere while nitric acid dominated in the lower troposphere. Peroxynitric acid (HO2NO2) was present in sizable concentrations always peaking at around 8 km. Aerosol nitrate appeared to be mostly contained in large soil based particles in the lower troposphere. Plumes from Alaskan fires contained large amounts of PAN and very little enhancement in ozone. Observational data suggest that lightning was a far greater contributor to NO(x) in the upper troposphere than previously believed. NO(x) and NO(y) reservoir appeared to be in steady state only in the middle troposphere where NO(x)/NO(y) was independent of air mass age. A first comparison of observed data with simulations from four 3-D models shows significant differences between observations and models as well as among models. These uncertainties likely propagate themselves in satellites derived NOx data. Observed data are interpreted to suggest that soil sinks of HCN/CH3CN are at best very small. 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.↗

Ozone and Water Vapor Measurements by Raman Lidar in the Planetary Boundary Layer: Error Sources and Field Measurements

Why do we need time series of ozone and water vapor profiles at low altitude? The degradation of air quality is a very serious environmental problem that affects urban and industrial areas worldwide. Air pollution injures human health and ecosystems, diminishes crop yield, and spoils patrimony and materials. The phenomena involved in air pollution are very complex. Once emitted into the atmosphere, (primary) pollutants are transported, dispersed, transformed by gas/solid phase change and chemical reaction, and finally removed by dry and wet deposition. Most challenging is the fact that the health and environmental impacts of secondary pollutants (formed in the atmosphere) are frequently more severe than those of their precursors (primary pollutants). This is the case of ozone and other photochemical pollutants, such as peroxyacetil nitrate (PAN) and secondary particles, produced in the atmosphere by the photo-oxidation volatile organic compounds (VOC) catalyzed by nitrogen oxides (NO(sub x)). Photochemical air pollution is a complex science because of the non-linearity of its response to changes in primary emission.

Lazzarotto, Benoit↗

Insights into Tropospheric Ozone from the INTEX Ozonesonde Network Study (IONS)

Ozone profile data from soundings integrate models, aircraft and other ground-based measurements for better interpretation of atmospheric chemistry and dynamics. A well-designed network of ozonesonde stations, with consistent sampling, can answer questions not possible with short campaigns or current satellite technology. The SHADOZ (Southern Hemisphere Additional Ozonesondes) project, for example, has led to these findings about tropical ozone: definition of the zonal tropospheric wave-one pattern in equatorial ozone, characterization of the "Atlantic ozone paradox" and establishment of a link between tropical Atlantic and Indian Ocean pollution. Building on the SHADOZ concept, a short-term ozone network was formed in July-August 2004 to coordinate ozonesonde launches during the ICARTT/INTEX/NEAQS (International Consortium on Atmospheric Research on Transport and Transformation)/Intercontinental Transport Experiment/New England Air Quality Study. In IONS (INTEX Ozonesonde Network Study), more than 250 soundings, with daily frequency at half the sites, were launched from eleven North American stations and an oceanographic ship in the Gulf of Maine. Although the goal was to examine pollution influences under stable high-pressure systems and transport associated with "warm conveyor belt" flows, the INTEX study region was dominated by a series of weak frontal system that mixed aged pollution with stratospheric ozone in the middle troposphere. Deconvoluting ozone sources provides new insights into ozone in the transition between mid-latitude and polar air.

Thompson, Anne M.↗

Intercontinental Transport of Tropical Ozone from Biomass Burning: Views from Satellite and SHADOZ (Southern Hemisphere Additional Ozonesondes)

There has been interest in the connection between tropical fires and ozone since about 1980. Photochemically reactive gases released by fires (e.g. NO, CO, volatile organic carbon) interact as they do in an urban environment to form ozone. Interacting with chemical sources, tropical meteorology plays a part in tropospheric ozone distributions in the tropics, through large-scale circulation, deep convection, and regional phenomena like the West African and Asian monsoons. An overview of observations, taken from satellite and from ozone soundings, illustrates regional influences and intercontinental- range ozone transport in the tropics. One of the most striking findings is evidence for impacts of Indian Ocean pollution on the south Atlantic ozone maximum referred to as the "ozone paradox" [Thompson et al., GRL, 2000; JGR, 2003; Chatfield et al., GRL, 20031.

Thompson, A. M.↗

NASA advanced aeronautics design solar powered remotely piloted vehicle

Environmental problems such as the depletion of the ozone layer and air pollution demand a change in traditional means of propulsion that is sensitive to the ecology. Solar powered propulsion is a favorable alternative that is both ecologically harmless as well as cost effective. Integration of solar energy into designs ranging from futuristic vehicles to heating is beneficial to society. The design and construction of a Multi-Purpose Remotely Piloted Vehicle (MPRPV) seeks to verify the feasibility of utilizing solar propulsion as a primary fuel source. This task has been a year long effort by a group of ten students, divided into five teams, each dealing with different aspects of the design. The aircraft was designed to take-off, climb to the design altitude, fly in a sustained figure-eight flight path, and cruise for approximately one hour. This mission requires flight at Reynolds numbers between 150,000 and 200,000 and demands special considerations in the aerodynamic design in order to achieve flight in this regime. Optimal performance requires a light weight configuration with both structural integrity and maximum power availability. The structure design and choice of solar cells for the propulsion was governed by the weight, efficiency, and cost considerations. The final design is a MPRPV weighting 35 N which cruises 7 m/s at the design altitude of 50 m. The configuration includes a wing composed of balsa and foam NACA 6409 airfoil sections and carbon fiber spars, a tail of similar construction, and a truss structure fuselage. The propulsion system consists of 98 10 percent efficient solar cells donated by Mobil Solar, a NiCad battery for energy storage, and a folding propeller regulated by a lightweight and efficient control system. The airfoils and propeller chosen for the design were research and tested during the design process.

Elario, David S.↗

Solar powered multipurpose remotely powered aircraft

Environmental problems such as the depletion of the ozone layer and air pollution demand a change in traditional means of propulsion that is sensitive to the ecology. Solar-powered propulsion is a favorable alternative that is both ecologically harmless as well as cost effective. Integration of solar energy into designs ranging from futuristic vehicles to heating is, therefore, beneficial to society. The design and construction of a Multipurpose Remotely Piloted Vehicle (MPRPV) seeks to verify the feasibility of using solar propulsion as a primary fuel source. This task has been a year-long effort by a group of eight students, divided into four teams, each dealing with different aspects of the design. The aircraft was designed to take off, climb to the design altitude, fly in a sustained figure-eight flight path, and cruise for approximately one hour. This mission requires flight at Reynolds numbers between 150,000 and 200,000 and demands special considerations in the aerodynamic design to achieve flight in this regime. Optimal performance requires a lightweight configuration with both structural integrity and maximum power availability. The structural design and choice of solar cells for the propulsion were governed by weight, efficiency, and cost considerations. The final design is an MPRPV weighing 35 N that cruises at 7 m/s at the design altitude of 50 m. The configuration includes a wing composed of balsa and foam NACA 6409 airfoil sections and carbon fiber spars, a tail of similar construction, and a truss structure fuselage. The propulsion system consists of 98 12.5 percent-efficient solar cells donated by Mobil Solar, a NiCad battery for energy storage, and a folding propeller regulated by a lightweight and efficient control system. The airfoils and propeller chosen for the design were researched and tested during the design process.

Source record↗

ATLAS-2 Video News Release

This NASA Kennedy Space Center (KSC) video presents a Marshall Space Flight Center-Television (MSFC-TV) news release describing the objectives of the Atmospheric Laboratory for Applications in Science-2 (ATLAS-2), which is being flown on STS-56. Dr. Tim Miller (Mission Scientist), Dr. Marsha Torr (Mission Scientist), and Teresa Vanhooser (Mission Manager) explain that the ATLAS-2 mission is being launched to study earth atmospheric interactions with the sun in general and how manmade chemicals and pollution are contributing to ozone depletion in our atmosphere in particular. Seven instruments comprise the core payload. ATLAS-2 is an integral part of the Spacelab contribution to NASA's Mission to Planet Earth and characterizes the chemical and physical components of Earth's middle atmosphere and the solar energy injected in the atmosphere, studies that began on ATLAS-1.

Source record↗

Measurements of Long-Lived Trace Gases from Commercial Aircraft Platforms: Development of Instrumentation

The upper troposphere (6-12 km altitude) is a poorly understood and highly vulnerable region of the atmosphere. It is important because many trace species, including ozone, have their greatest impact as greenhouse (infrared-absorbing) gases in this region. The addition of relatively small amounts of anthropogenic chemicals, such as nitrogen oxides, can have a dramatic effect on the abundance of ozone. Some of these pollutants are deposited directly, e.g., by aircraft, while others are transported in. The primary goal of this project was to measure several chemical compounds in the upper troposphere that will help us to understand how air is to transported to that part of the atmosphere; that is, does it come down from the stratosphere, does it rise from the surface via convection, and so on. To obtain adequate sampling to accomplish this goal, we proposed to make measurements from revenue aircraft during normal flight operations.

Source record↗

Airborne In-Situ Measurements of Formaldehyde Over California: One Year of Results from the Compact Formaldehyde Fluorescence Experiment (COFFEE) Instrument

Formaldehyde (HCHO) is one of the most abundant oxygenated volatile organiccompounds (VOCs) in the atmosphere, playing a role in multiple atmosphericprocesses, such as ozone (O3) production in polluted environments. Due toits short lifetime of only a few hours in daytime, HCHO also serves astracer of recent photochemical activity. While photochemical oxidation ofnon-methane hydrocarbons is the dominant source, HCHO can also be emitteddirectly from fuel combustion, vegetation, and biomass burning. The CompactFormaldehyde FluorescencE Experiment (COFFEE) instrument was built forintegration onto the Alpha Jet Atmospheric eXperiment (AJAX) payload, basedout of NASAs Ames Research Center (Moffett Field, CA). Using Non-ResonantLaser Induced Fluorescence (NR-LIF), trace concentrations of HCHO can bedetected with a sensitivity of 200 parts per trillion.Since its first research flight in December 2015, COFFEE has successfullyflown on more than 20 science missions throughout California and Nevada.Presented here are results from these flights, including boundary layermeasurements and vertical profiles throughout the tropospheric column.Californias San Joaquin Valley is a primary focus, as this region is knownfor its elevated levels of HCHO as well as O3. Measurements collected inwildfire plumes, urban centers, agricultural lands, and on and off shorecomparisons will be presented. In addition, the correlation of HCHO to othertrace gases also measured by AJAX, including O3, methane, carbon dioxide,and water vapor will also be shown. Lastly, the implications of these HCHOmeasurements on calibration and validation of remote sensing data collectedby NASAs OMI (Aura) and OMPS (SuomiNPP) satellites will be addressed.

wildfire↗

Convective Distribution of Tropospheric Ozone and Tracers in the Central American ITCZ Region: Evidence from Observations During TC4

During the Tropical Composition, Clouds and Climate Coupling (TC4) experiment that occurred in July and August of 2007, extensive sampling of active convection in the ITCZ region near Central America was performed from multiple aircraft and satellite sensors. As part of a sampling strategy designed to study cloud processes, the NASA ER-2, WB-57 and DC-8 flew in stacked "racetrack patterns" in convective cells. On July 24, 2007, the ER-2 and DC-8 probed an actively developing storm and the DC-8 was hit by lightning. Case studies of this flight, and of convective outflow on August 5, 2007 reveal a significant anti-correlation between ozone and condensed cloud water content. With little variability in the boundary layer and a vertical gradient, low ozone in the upper troposphere indicates convective transport. Because of the large spatial and temporal variability in surface CO and other pollutants in this region, low ozone is a better convective indicator. Lower tropospheric tracers methyl hydrogen peroxide, total organic bromine and calcium substantiate the ozone results. OMI measurements of mean upper tropospheric ozone near convection show lower ozone in convective outflow. A mass balance estimation of the amount of convective turnover below the tropical tropopause transition layer (TTL) is 50%, with an altitude of maximum convective outflow located between 10 and 11 km, 4 km below the cirrus anvil tops. It appears that convective lofting in this region of the ITCZ is either a two-stage or a rapid mixing process, because undiluted boundary layer air is never sampled in the convective outflow.

Avery, Melody↗

Has NO(2) in Metropolitan Areas Returned to Pre-COVID-19 Levels as Measured by OMI Satellite Data?

Nitrogen oxides (NOx = NO + NO2) are primarily emitted through the combustion of fossil fuels, such as automobiles and power plants. NOx can contribute to chemical reactions that produce ozone and fine particulate matter (PM2.5) pollution. Using tropospheric vertical column density (TVCD) NO2 data from satellite hyperspectral instruments, such as the Ozone Monitoring Instrument (OMI) on board NASA’s EOS Aura satellite, one can monitor changes in NO2 pollution during “black-swan” events, such as mobility restrictions during COVID-19 lockdowns. Our OMI team has created the Global Nitrogen Dioxide Monitoring Home Page (https://so2.gsfc.nasa.gov/no2/no2_index.html ) where we display NO2 TVCD time series, animated maps, and COVID-specific NO2 anomalies comparing to a pre-COVID five-year average for 317 cities and regions around the world. During the pandemic as a result of the widespread lockdowns, many areas saw low NO2 anomalies superimposed on the natural weather related NO2 changes, such as seasonal NO2 cycle. Has NO2 levels returned to pre-Covid-19 levels in large metropolitan areas? We analyze NO2 time series from March through September for the years 2020-2023 using as a reference the average NO2 from 2015-2019 for those months. We will present data from selected cities that represent all countries.

Keith D Evans↗

Comparison of ozone determinations by ultraviolet photometry and gas-phase titration

A comparison of ozone determinations based on ultraviolet absorption photometry and gas-phase titration (GPT) shows good agreement between the two methods. Together with other results, these findings indicate that three candidate reference methods for ozone, UV photometry, IR photometry, and GPT are in substantial agreement. However, the GPT method is not recommended for routine use by air pollution agencies for calibration of ozone monitors because of susceptibility to experimental error.

Demore, W. B.↗

Climate Change Penalty and Benefit on Surface Ozone: A Global Perspective Based on CMIP6 Earth System Models

This work presents an analysis of the effect of climate change on surface ozone discussing the related penalties and benefits around the globe from the global modelling perspective based on simulations with five CMIP6 (Coupled Model Intercomparison Project Phase 6) Earth System Models. As part of AerChemMIP (Aerosol Chemistry Model Intercomparison Project) all models conducted simulation experiments considering future climate (ssp370SST) and present-day climate (ssp370pdSST) under the same future emissions trajectory (SSP3-7.0). A multi-model global average climate change benefit on surface ozone of −0.96 ± 0.07 ppbv °C−1 is calculated which is mainly linked to the dominating role of enhanced ozone destruction with higher water vapour abundances under a warmer climate. Over regions remote from pollution sources, there is a robust decline in mean surface ozone concentration on an annual basis as well as for boreal winter and summer varying spatially from −0.2 to −2 ppbv °C−1, with strongest decline over tropical oceanic regions. The implication is that over regions remote from pollution sources (except over the Arctic) there is a consistent climate change benefit for baseline ozone due to global warming. However, ozone increases over regions close to anthropogenic pollution sources or close to enhanced natural biogenic volatile organic compounds emission sources with a rate ranging regionally from 0.2 to 2 ppbv C−1, implying a regional surface ozone penalty due to global warming. Overall, the future climate change enhances the efficiency of precursor emissions to generate surface ozone in polluted regions and thus the magnitude of this effect depends on the regional emission changes considered in this study within the SSP3_7.0 scenario. The comparison of the climate change impact effect on surface ozone versus the combined effect of climate and emission changes indicates the dominant role of precursor emission changes in projecting surface ozone concentrations under future climate change scenarios.

surface ozone↗