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Intercontinental Transport of Air Pollution

The development of the global economy goes beyond raising our standards of living. We are in an ear of increasing environmental as well as economic interdependence. Long-range transport of anthropogenic atmospheric pollutants such as ozone, ozone precursors, airborne particles, heavy metals (such as mercury) and persistent organic pollutants are the four major types of pollution that are transported over intercontinental distances and have global environmental effects. The talk includes: 1) an overview of the international agreements related to intercontinental transport of air pollutants, 2) information needed for decision making, 3) overview of the past research on intercontinental transport of air pollutants - a North American's perspective, and 4) future research needs.

Rogers, David↗

Field Calibration Techniques used to Characterize the Radiometric Stability of the GEO-CAPE Airborne Simulator (GCAS)

The GEOstationary Coastal and Air Pollution Events (GEO-CAPE) Airborne Simulator (GCAS) was developed at NASA’s Goddard Space Flight Center (GSFC) and has flown in multiple field campaigns to perform mapping of the regional-scale EPA criteria pollutants nitrogen dioxide, ozone, and formaldehyde. GCAS will also participate invalidation campaigns for NASA’s Tropospheric Emissions: Monitoring POllution (TEMPO) mission and the Korean Geostationary Environment Monitoring Spectrometer (GEMS) mission, both scheduled to launch in the early 2020s. GCAS houses two commercial Offner-type grating spectrometers that measure backscattered solar spectral radiance from the near-ultraviolet to near-infrared at high spatial resolution (typically 250 meters at 8.5 kilometer altitude). These radiances are used to retrieve spatial and temporal distributions of trace gases relevant to the boundary layer and free tropospheric atmospheric chemistry cycles. In this paper, we describe the field calibration techniques employed to characterize the spectral and temporal radiometric stability of the system during its most recent deployment in the 2018 Long Island Sound Trace Ozone Study (LISTOS) field campaign. Overall measurement uncertainty, retrieval impacts, and lessons learned for future deployments will also be described.

NASA’s Tropospheric Emissions: Monitoring POllutio↗

Aura OMI Observations of Regional SO2 and NO2 Pollution Changes from 2005 to 2015

The Ozone Monitoring Instrument (OMI) onboard NASA's Aura satellite has been providing global observations of the ozone layer and key atmospheric pollutant gases, such as nitrogen dioxide (NO2) and sulfur dioxide (SO2), since October 2004. The data products from the same instrument provide consistent spatial and temporal coverage and permit the study of anthropogenic and natural emissions on local-to-global scales. In this paper, we examine changes in SO2 and NO2 over some of the world's most polluted industrialized regions during the first decade of OMI observations. In terms of regional pollution changes, we see both upward and downward trends, sometimes in opposite directions for NO2 and SO2, for different study areas. The trends are, for the most part, associated with economic and/or technological changes in energy use, as well as regional regulatory policies. Over the eastern US, both NO2 and SO2 levels decreased dramatically from 2005 to 2015, by more than 40 and 80 percent, respectively, as a result of both technological improvements and stricter regulations of emissions. OMI confirmed large reductions in SO2 over eastern Europe's largest coal-fired power plants after installation of flue gas desulfurization devices. The North China Plain has the world's most severe SO2 pollution, but a decreasing trend has been observed since 2011, with about a 50 percent reduction in 2012-2015, due to an economic slowdown and government efforts to restrain emissions from the power and industrial sectors. In contrast, India's SO2 and NO2 levels from coal power plants and smelters are growing at a fast pace, increasing by more than 100 and 50 percent, respectively, from 2005 to 2015. Several SO2 hot spots observed over the Persian Gulf are probably related to oil and gas operations and indicate a possible underestimation of emissions from these sources in bottom-up emission inventories. Overall, OMI observations have proved valuable in documenting rapid changes in air quality over different parts of the world during last decade. The baseline established during the first 11 years of OMI is indispensable for the interpretation of air quality measurements from current and future satellite atmospheric composition missions.

SO2 and NO2↗

Aura OMI observations of regional SO2 and NO2 pollution changes from 2005 to 2015

The Ozone Monitoring Instrument (OMI) onboard NASA's Aura satellite has been providing global observations of the ozone layer and key atmospheric pollutant gases, such as nitrogen dioxide (NO2/ and sulfur dioxide (SO2/, since October 2004. The data products from the same instrument provide consistent spatial and temporal coverage and permit the study of anthropogenic and natural emissions on local-to-global scales. In this paper, we examine changes in SO2 and NO2 over some of the world's most polluted industrialized regions during the first decade of OMI observations. In terms of regional pollution changes, we see both upward and downward trends, sometimes in opposite directions for NO2 and SO2, for different study areas. The trends are, for the most part, associated with economic and/or technological changes in energy use, as well as regional regulatory policies. Over the eastern US, both NO2 and SO2 levels decreased dramatically from 2005 to 2015, by more than 40 and 80 %, respectively, as a result of both technological improvements and stricter regulations of emissions. OMI confirmed large reductions in SO2 over eastern Europe's largest coal-fired power plants after installation of flue gas desulfurization devices. The North China Plain has the world's most severe SO2 pollution, but a decreasing trend has been observed since 2011, with about a 50% reduction in 2012- 2015, due to an economic slowdown and government efforts to restrain emissions from the power and industrial sectors. In contrast, India's SO2 and NO2 levels from coal power plants and smelters are growing at a fast pace, increasing by more than 100 and 50 %, respectively, from 2005 to 2015. Several SO2 hot spots observed over the Persian Gulf are probably related to oil and gas operations and indicate a possible underestimation of emissions from these sources in bottom-up emission inventories. Overall, OMI observations have proved valuable in documenting rapid changes in air quality over different parts of the world during last decade. The baseline established during the first 11 years of OMI is indispensable for the interpretation of air quality measurements from current and future satellite atmospheric composition missions.

Pollution trends↗

Vertical Profiling of Air Pollution at RAPCD

The interaction between local and regional pollution levels occurs at the interface of the Planetary Boundary Layer and the Free Troposphere. Measuring the vertical distribution of ozone, aerosols, and winds with high temporal and vertical resolution is essential to diagnose the nature of this interchange and ultimately for accurately forecasting ozone and aerosol pollution levels. The Regional Atmospheric Profiling Center for Discovery, RAPCD, was built and instrumented to address this critical issue. The ozone W DIAL lidar, Nd:YAG aerosol lidar, and 2.1 micron Doppler wind lidar, along with balloon- borne ECC ozonesondes form the core of the W C D instrumentation for addressing this problem. Instrumentation in the associated Mobile Integrated Profiling (MIPS) laboratory includes 91 5Mhz profiler, sodar, and ceilometer. The collocated Applied particle Optics and Radiometry (ApOR) laboratory hosts an FTIR along with MOUDI and optical particle counters. With MODELS-3 analysis by colleagues in the National Space Science and Technology Center on the UAH campus and the co- located National Weather Service Forecasting Office in Huntsville, AL we are developing a unique facility for advancing the state of the science of pollution forecasting.

Newchurch, Michael J.↗

Assessment and Applications of NASA Ozone Data Products Derived from Aura OMI-MLS Satellite Measurements in Context of the GMI Chemical Transport Model

Measurements from the Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS), both onboard the Aura spacecraft, have been used to produce daily global maps of column and profile ozone since August 2004. Here we compare and evaluate three strategies to obtain daily maps of tropospheric and stratospheric ozone from OMI and MLS measurements: trajectory mapping, direct profile retrieval, and data assimilation. Evaluation is based upon an assessment that includes validation using ozonesondes and comparisons with the Global Modeling Initiative (GMI) chemical transport model (CTM). We investigate applications of the three ozone data products from near-decadal and inter-annual timescales to day-to-day case studies. Zonally averaged inter-annual changes in tropospheric ozone from all of the products in any latitude range are of the order 1-2 Dobson Units while changes (increases) over the 8-year Aura record investigated http://eospso.gsfc.nasa.gov/atbd-category/49 vary approximately 2-4 Dobson Units. It is demonstrated that all of the ozone products can measure and monitor exceptional tropospheric ozone events including major forest fire and pollution transport events. Stratospheric ozone during the Aura record has several anomalous inter-annual events including stratospheric warming split events in the Northern Hemisphere extra-tropics that are well captured using the data assimilation ozone profile product. Data assimilation with continuous daily global coverage and vertical ozone profile information is the best of the three strategies at generating a global tropospheric and stratospheric ozone product for science applications.

GMI↗

A Madden-Julian Oscillation in Tropospheric Ozone

This is the first study to indicate a Madden-Julian Oscillation (MJO) in tropospheric ozone. Tropospheric ozone is derived using differential measurements of total column ozone and stratospheric column ozone measured from total ozone mapping spectrometer (TOMS) and microwave limb sounder (MLS) instruments. Two broad regions of significant MJO signal are identified in the tropics, one in the western Pacific and the other in the eastern Pacific. Over both regions, MJO variations in tropospheric ozone represent 5-10 Dobson Unit (DU) peak-to-peak anomalies. These variations are significant compared to mean background amounts of 20 DU or less over most of the tropical Pacific. MJO signals of this magnitude would need to be considered when investigating and interpreting particular pollution events since ozone is a precursor of the hydroxyl (OH) radical, the main oxidizing agent of pollutants in the lower atmosphere.

Ziemke, J. R.↗

Convective Transport to the Upper Troposphere and Lower Stratosphere Over the Asian Summer Monsoon as Observed During the 2022 ACCLIP Airborne Campaign

Deep convection in the Asian summer monsoon (ASM) rapidly transports boundary layer pollutants including ozone-depleting substances into the upper troposphere and lower stratosphere (UTLS). The confinement of the seasonal anticyclonic circulation in the UTLS over Asia initially traps the pollutants near the tropopause level, but air masses are subsequently transported throughout the global stratosphere and impact Earth’s climate. Characterizing the transport pathways and processes of these pollutants are critical for identifying source regions and quantifying regional contributions to global stratospheric concentrations. The Asian summer monsoon Chemical and Climate Impact Project (ACCLIP) was conducted in summer 2022 using two high-altitude aircraft (NSF NCAR Gulfstream V and the NASA WB-57) to obtain UTLS chemical composition and aerosol distribution for characterizing the impact of the ASM on global chemistry and climate. Backward trajectories from ACCLIP flight tracks were traced through time-varying, satellite-derived global convective cloud top altitude fields to investigate the convective air mass origins of the sampled air parcels. Analyses reveal that air masses lofted by convection within the ASM (South Asian summer monsoon) and near the edge of the of the ASM anticyclone (East Asian summer monsoon) contributed to the airborne observations. In this study, we present a summary of the transport statistics of UTLS air masses sampled during ACCLIP and discuss the implications of these results on our understanding of the role of ASM in global constituent transport.

Convective↗

History of Ozone Research: From Schonbein to the Present

In 1840, C.F. Schonbein recognized that the smell generated in several different electrical and chemical processes was a single substance. He named this substance "ozein" from the Greek for "to smell". This substance we know today as ozone. Several periods can be distinguished in the continued development of our understanding of ozone. Throughout the late 19th century, the identity and properties of ozone were established and described. Ozone was recognized to be a constituent of normal air and tests were established to measure its concentration. Its disinfectant properties were recognized. New methods were developed for making ozone in the laboratory. In 1879, ultraviolet spectroscopic techniques were applied to the measurement of the solar spectrum and it was discovered by Comu that the spectrum was cut off at about 300 nm wavelength. Hartley suggested, based on laboratory measurements, that this cutoff was due to ozone in the atmosphere which he correctly asserted was somewhere in the upper atmosphere. This began the period of development of the amount and distribution of ozone throughout the atmosphere. In 1930, Chapman put forward the first theory of the formation and destruction of ozone. By the mid-1960s it was becoming obvious that the description of the chemical loss term was inadequate. By the early 1970s the chemical destruction of ozone by the oxides of hydrogen, nitrogen, chlorine, and bromine was recognized as an essential element in the chemical balance determining the ozone concentration. Today, ozone is a broad research project which crosses the boundaries of traditional disciplines. Stratospheric ozone loss due to chlorofluorocarbons is a newsworthy item. The Antarctic ozone hole opens up every spring. The provisions of the Montreal Protocol were agreed upon by countries around the world and promise to reduce the future levels of ozone-destroying chlorine in the stratosphere. Ozone concentrations in polluted cities are a subject of local and national regulations to limit its potential for causing health problems and corrosive effects on materials. A lot is known about ozone but many new questions are still being developed.

Stolarski, Richard S.↗

Consequences of Insufficient Production of Temporary NOx Reservoirs on Ozone Production in Models During KORUS-AQ

The advent of geostationary satellites, starting with GEMS over South Korea, offer the potential for additional insight into urban air quality. In preparation for these satellites, the joint NIER-NASA KORUS-AQ field campaign in 2016 obtained a large dataset for understanding local air quality and the contribution of local emissions to ozone and PM2.5 pollution. Models partitioned NOx primarily into inorganic nitrate (HNO3 + nitrate aerosol) while observations suggest that acyl peroxy nitrates (PNs) should be an important sink. Models tended to produce ozone too efficiently, which may be due to insufficient alkyl/multifunctional nitrate (ANs) production. Models are unable to simulate the transport of NOx away from the urban center and its impact on ozone production downwind.

Katherine R Travis↗

Local to Global Air Quality Simulations using the NASA GEOS Composition Forecast Model, GEOS-CF

We give an overview of the NASA Global Earth Observing System Composition Forecast model (GEOS-CF), a high-resolution (roughly 25-km) global composition model developed by the NASA Global Modeling and Assimilation Office (GMAO). This system combines the GEOS weather and aerosol model with the GEOS-Chem chemistry module to provide a holistic view of atmospheric composition that captures a wide range of air pollutants such as ozone,nitrogen oxides, volatile organic compounds, and fine particulate matter.Given the global extent of the model, GEOS-CF captures large-scale processes such as long-range transport of air pollutants, across ocean basins and continents.

Knowland, Emma K.↗

A Madden-Julian Oscillation in Tropospheric Ozone

This is the first study to indicate a Madden-Julian Oscillation (MJO) in tropospheric ozone. Tropospheric ozone is derived using differential measurements of total column ozone and stratospheric column ozone measured from total ozone mapping spectrometer (TOMS) and microwave limb sounder (MLS) instruments. Two broad regions of significant MJO signal are identified in the tropics, one in the western Pacific and the other in the eastern Pacific. Over both regions, MJO variations in tropospheric ozone represent 5- 10 DU peak-to-peak anomalies. These variations are significant compared to mean background amounts of 20 DU or less over most of the tropical Pacific. The implications of these results are: (1) model values of TCO in the tropical Pacific region, when accounted for the MJO may be highly variable depending upon the phase of the MJO, and (2) MJO signals of this magnitude would need to be considered when investigating and interpreting particular pollution events since ozone is a precursor of the hydroxyl (OH) radical, the main oxidizing agent of pollutants in the lower atmosphere.

Ziemke, J. R.↗

Gas-Phase Formation Rates of Nitric Acid and Its Isomers Under Urban Conditions

Ozone formation in urban smog is controlled by a complex set of reactions which includes radical production from photochemical processes, catalytic cycles which convert NO to NO2, and termination steps that tie up reactive intermediates in long-lived reservoirs. The reaction OH + NO2 + M -4 HONO2 + M (la) is a key termination step because it transforms two short-lived reactive intermediates, OH and NO2, into relatively long-lived nitric acid. Under certain conditions (low VOC/NOx), ozone production in polluted urban airsheds can be highly sensitive to this reaction, but the rate parameters are not well constrained. This report summarizes the results of new laboratory studies of the OH + NO2 + M reaction including direct determination of the overall rate constant and branching ratio for the two reaction channels under atmospherically relevant conditions.

Air pollution↗

Southeast Michigan Health & Air Quality: Identifying Trends of Ground-level Ozone Precursors in Southeast Michigan and Northern Ohio

Pollutants resulting from industrial activity can react with sunlight to create ground-level ozone, a harmful pollutant that can exacerbate respiratory health issues such as asthma. Due to a history of heavy industrialization, residents of southeast Michigan and northern Ohio are especially susceptible to ground-level ozone. NASA DEVELOP, in partnership with the Michigan Department of Environment, Great Lakes, and Energy’s (EGLE) Air Quality Division and the Lake Michigan Air Directors Consortium (LADCO), investigated the effectiveness of Earth observations (EO) in monitoring pollutants that contribute to ground-level ozone. The team used the European Space Agency’s TROPOspheric Monitoring Instrument (TROPOMI) aboard Sentinel-5P, and NASA’s Ozone Monitoring Instrument (OMI) aboard Aura, to measure nitrogen dioxide (NO2), formaldehyde (HCHO), and methane (CH4) from 2019 to 2021 (May-September). The team oversampled the EO data on monthly, yearly, and 3-year time scales where possible to enhance more localized pollutant trends. Specifically, TROPOMI effectively monitored NO2 from space, indicating sub-city distributions on a monthly timescale. Contrastingly, the measurements of HCHO were predominately noisy, and therefore failed to show any distribution trends. Lastly, CH4 trends were identifiable yet coarse, hinting that EO monitoring in the case of CH4 is not beneficial for our partners. The end products provide the partners with insight on the utility of EO in measuring certain ozone precursors and can be used to guide ground-level ozone reduction strategies throughout the region.

Mariam Moeen↗

The Central Role of Air Quality Observations in NASA's GEOS Composition Forecasting Model

The NASA GEOS composition forecast model (GEOS-CF) provides global, high-resolution (25 km) air quality forecasts in near-real time. This system combines the operational GEOS-5 weather forecasting model with the state-of-the-science GEOS-Chem chemistry module to provide detailed chemical analysis of a wide range of air pollutants such as ozone, carbon monoxide, nitrogen oxides, and fine particulate matter (PM2.5). The resolution of the forecasts is the highest compared to current, publicly-available global composition forecasts.Air quality observations are an indispensable tool to evaluate the model's ability to capture the strong temporal and spatial gradients of air pollutants across the globe. We show how comparisons against near-real time observations available through OpenAQ (www.openaq.org) demonstrate the model's overall success in reproducing surface concentrations of ozone, nitrogen dioxide, and PM2.5. This analysis also helps identifying current limitations of the model, for example over South America. The model-observation mismatches are most likely caused by uncertainties in the emissions data. Using the example of Rio de Janeiro, we show how the model skill can be improved by using local, high-resolution emission inventories in combination with air quality data.

Keller, Christoph A.↗

High Resolution Global Coupled Chemistry-Meteorology Simulations Using the NASA GEOS Composition Forecast System, GEOS-CF

We will give an overview of the NASA Global Earth Observing System Composition Forecast system (GEOS-CF), a high-resolution (0.25 degree) global composition model developed by the NASA Global Modeling and Assimilation Office (GMAO). This system combines the GEOS weather and aerosol model with the GEOS-Chem chemistry module (version 12) to provide a holistic view of atmospheric composition that captures a wide range of air pollutants such as ozone, nitrogen oxides, volatile organic compounds, and fine particulate matter. The spatial resolution of 0.25 degrees (approx. 25 km) is fine enough to resolve local features such as nighttime ozone titration previously resolved only by urban or regional models. Furthermore, since there are no boundary conditions for a global model, the GEOS-CF captures large-scale processes such as long-range transport of air pollutants from forest fires. Comparisons against surface observations highlight the model’s overall capability to reproduce the diurnal variability of air pollutants under a variety of meteorological conditions. In addition, we show how machine learning techniques can be used to correct for sub-grid variability, which further improves model estimates at a given surface observation site. The GEOS-CF system offers a new tool for scientists and the public health community alike and is being developed jointly with several government and non-profit partners. As an example, we will show the use of GEOS-CF during the Satellite Coastal and Oceanic Atmospheric Pollution Experiment (SCOAPE). The campaign, conducted in collaboration between NASA and the Bureau of Ocean Energy Management (BOEM), aims to investigate the response of onshore air quality to Outer Continental Shelf (OCS) oil and gas exploration, development and production. Detailed gas-phase chemistry, as provided by GEOS-CF, is critical to understand the formation of air pollution related to hydrocarbon emissions from offshore oil and gas activities. The accuracy of GEOS-CF can be further improved by incorporating detailed offshore emissions compiled by BOEM.

Knowland, K. Emma↗

Evaluating the Impact of Chemical Complexity and Horizontal Resolution on Tropospheric Ozone Over the Conterminous US With a Global Variable Resolution Chemistry Model

A new configuration of the Community Earth System Model (CESM)/Community Atmosphere Model with full chemistry (CAM-chem) supporting the capability of horizontal mesh refinement through the use of the spectral element (SE) dynamical core is developed and called CESM/CAM-chem-SE. Horizontal mesh refinement in CESM/CAM-chem-SE is unique and novel in that pollutants such as ozone are accurately represented at human exposure relevant scales while also directly including global feedbacks. CESM/CAM-chem-SE with mesh refinement down to ∼14 km over the conterminous US (CONUS) is the beginning of the Multi-Scale Infrastructure for Chemistry and Aerosols (MUSICAv0). Here MUSICAv0 is evaluated and used to better understand how horizontal resolution and chemical complexity impact ozone and ozone precursors over CONUS as compared to measurements from five aircraft campaigns, which occurred in 2013. This field campaign analysis demonstrates the importance of using finer horizontal resolution to accurately simulate ozone precursors such as nitrogen oxides and carbon monoxide. In general, the impact of using more complex chemistry on ozone and other oxidation products is more pronounced when using finer horizontal resolution where a larger number of chemical regimes are resolved. Large model biases for ozone near the surface remain in the Southeast US as compared to the aircraft observations even with updated chemistry and finer horizontal resolution. This suggests a need for adding the capability of replacing sections of global emission inventories with regional inventories, increasing the vertical resolution in the planetary boundary layer, and reducing model biases in meteorological variables such as temperature and clouds.

MUSICA↗