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NASA NTRS2021

Impact of Regional Northern Hemisphere Mid-latitude Anthropogenic Sulfur Dioxide Emissions on Local and Remote Tropospheric Oxidants

The unintended consequences of reductions in regional anthropogenic sulfur dioxide (SO2) emissions implemented to protect human health are poorly understood. SO2 decreases began in the 1970s in the US and Europe and are expected to continue into the future, while recent emissions decreases in China are also projected to continue. In addition to the well-documented climate effects (warming) from reducing aerosols, tropospheric oxidation is impacted via aerosol modification of photolysis rates and radical sinks. Impacts on the hydroxyl radical and other trace constituents directly affect climate and air quality metrics such as surface ozone levels. We use the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 nudged towards National Centers for Environmental Prediction (NCEP) reanalysis wind velocities to estimate the impact of SO2 emissions from the US, Europe, and China by differencing a control simulation with an otherwise identical simulation in which 2015 anthropogenic SO2 emissions are set to zero over one of the regions. Springtime sulfate aerosol changes occur both locally to the emission region and also throughout the Northern Hemispheric troposphere, including remote oceanic regions and the Arctic. Hydroperoxy (HO2) radicals are directly removed via heterogeneous chemistry on aerosol surfaces, including sulfate, in the model, and we find that sulfate aerosol produced by SO2 emissions from the three individual northern mid-latitude regions strongly reduces both HO2 and hydroxyl (OH) by up to 10 % year-round throughout most of the troposphere north of 30∘ N latitude. Regional SO2 emissions significantly increase nitrogen oxides (NOx) by about 5 %–8 % throughout most of the free troposphere in the Northern Hemisphere by increasing the NOx lifetime as the heterogeneous sink of HO2 on sulfate aerosol declines. Despite the NOx increases, tropospheric ozone decreases at northern mid-latitudes by 1 %–4 % zonally averaged and by up to 5 ppbv in summertime surface air over China, where the decreases in HO2 and OH suppress O3 production. Since 2015 anthropogenic SO2 emissions in China exceed those in the US or Europe, the oxidative response is greatest for the China perturbation simulation. Chemical effects of aerosols on oxidation (reactive uptake) dominate over radiative effects (photolysis rates), the latter of which are only statistically significant locally for the large perturbation over China. We find that the SO2 emissions decrease in China, which has yet to be fully realized, will have the largest impact on oxidants and related species in the Northern Hemisphere free troposphere compared to future decreases in Europe or the US. Our results bolster previous calls for a multipollutant strategy for air pollution mitigation to avoid the unintended consequence of aerosol removal leading to surface ozone increases that offset or mask surface ozone gains achieved by regulation of other pollutants, especially in countries where current usage of high-sulfur emitting fuels may be phased out in the future.

anthropogenic sulfur dioxide emissions↗
NASA NTRS1994

Modeling ozone episodes in the Baltimore-Washington region

Surface ozone (O3) concentrations in excess of the National Ambient Air Quality Standard (NAAQS) continue to occur in metropolitan areas in the United States despite efforts to control emissions of O3 precursors. Future O3 control strategies will be based on results from modeling efforts that have just begun in many areas. Two initial questions that arise are model sensitivity to domain-specific conditions and the selection of episodes for model evaluation and control strategy development. For the Baltimore-Washington region (B-W), the presence of the Chesapeake Bay introduces a number of issues relevant to model sensitivity. In this paper, the specific questions of the determination of model volume (mixing height) for the Urban Airshed Model (UAM) is discussed and various alternative methods compared. For the latter question, several analytic approaches, Cluster Analysis and classification and Regression Tree (CART) analysis are undertaken to determine meteorological conditions associated with severe O3 events in the B-W domain.

Ryan, William F.↗
NASA NTRS1991

Decrease of summer tropospheric ozone concentrations in Antarctica

It is shown here that surface ozone concentrations at the South Pole in the austral summer decreased by 17 percent over the period 1976-90. Over the same period, solar irradiance at the South Pole in January and February decreased by 7 percent as a result of a 25 percent increase in cloudiness. It is suggested that the trend in the summer ozone concentrations is caused by enhanced photochemical destruction of ozone in the lower troposphere caused by the increased penetration of UV radiation associated with stratospheric ozone depletion, coupled with enhanced transport of ozone-poor marine air from lower latitudes to the South Pole.

Schnell, R. C.↗
NASA NTRS1985

Tropospheric ozone - Seasonal behavior, trends, and anthropogenic influence

In the present analysis of tropospheric ozone data, attention is given to spatial and temporal variations. Two modes of seasonal behavior are noted for surface ozone at mid-latitudes: a broad summer maximum within a few hundred km of industrial/urban areas in Europe and the U.S., and a minimum in summer or autumn in sparcely populated regions that are remote from industrial activity. These and limited historical data indicate that summertime concentrations of ozone near the surface in the rural areas of Europe and the U.S. may have increased between 20 and 100 percent since the 1940s. It is suggested that the summer maximum in ozone and other observed trends are due to photochemical production associated with anthropogenic emissions of NO(x), hydrocarbons, and CO from fossil fuel combustion.

Logan, J. A.↗
NASA NTRS1994

Tropospheric ozone measurements at the equatorial region (1980-1988)

Results from surface ozone measurements at Penang (5.5 deg N, 100 deg E) over 1980-88 period are presented. The study indicates the ozone concentrations undergoing significant diurnal and seasonal variations. The peak concentration are observed at around mid-day (up to 35 nb) but the O3 concentration generally drops to zero level in the early evening and remains unchanged until mid-morning. Monthly-averaged daily 1-h average concentrations are generally small (4-13 nb) and decrease continually from the early part of the year to the end. Frequently, varying local weather conditions seem to influence the O3 concentrations.

Ilyas, Mohammad↗
NASA NTRS1999

Processes Affecting Tropospheric Ozone Inferred from Ozonesonde and Other Tracer Data from the R/V R H Brown Atlantic Cruise (37N-34S) in January-February 1999

During the Aerosols-99 trans-Atlantic cruise from Norfolk, VA, to Cape Town, South Africa, 22 ozonesondes were launched from the NOAA R/V R H Brown between 17 Jan and 6 Feb 1999, with all sondes but one reaching 30 km. A composite of ozone profiles along the transect shows high free tropospheric ozone (up to 100 ppbv at 9 km) between 5N and 20S, a coherent feature straddling either side of the ITCZ. Latitudinal variations of tropospheric ozone are interpreted using correlative measurements of surface ozone, CO, water vapor, and aerosol optical thickness (column absorbance) measured from the ship. Elevated ozone in the lower troposphere results from photochemical reactions of precursors emitted by biomass burning north of the ITCZ. However, the greatest ozone mixing ratios are in the mid-troposphere south of the ITCZ, which gives evidence of interhemispheric transport. Column-integrated tropospheric ozone, 35 DU from 0-16 km, agrees with that derived from the TOMS satellite by the modified-residual method [Thompson and Hudson, 1999]. NCEP wind fields, ship-launched radiosondes and back trajectories are consistent with a picture of recirculating air parcels centered in the tropical Atlantic region which is identified with the maximum wave-one amplitude in total ozone seen in sondes and by satellite.

Thompson, Anne M.↗
NASA NTRSDate not supplied

TPSAS-NF1676L-33873-DND

NOAA's National Air Quality Forecasting Capability (NAQFC) model provides 48-hour forecast of surface ozone and other atmospheric constituents serving as the nation's key tool actively used by regulatory professionals in assessing air quality events and the issuance of public air quality alerts. NAQFC incorporates input meteorology from North American Mesoscale Model (NAM) at 12 km horizontal resolution that is coupled to the Community Multi-scale Air Quality Model (CMAQ) to predict emissions, tropospheric gas and aerosol chemistry, and related deposition and removal processes. The NAQFC forecast simulations contain 35 steps in altitude, with about one third of these in a typical afternoon daytime boundary layer (0-1.5 km). While several studies have been conducted comparing NAQFC predictions to surface observations, investigations comparing the vertical distribution to observations remain limited. Vertical comparisons are needed in order to fully assess forecast model behavior and atmospheric mixing conditions leading to the formation of ozone at the surface. The Tropospheric Ozone Lidar Network (TOLNet) instruments provide a unique observational capability in this regard, as ozone vertical measurements can be directly compared to models, such as NAQFC, and provide additional insight into atmospheric processes and enhance forecast capabilities. In this study, we utilize multiple TOLNet lidar observations obtained during the Ozone Water Land Environmental Transition Studies (OWLETS-2017 & OWLETS-2018) and the Long Island Sound Tropospheric Ozone Study (LISTOS-2018) to compare with NAQFC vertical predictions of ozone. These campaigns took place at different coastal locations along the US East coast with each campaign having multiple TOLNet lidars present, providing a unique opportunity to examine vertical structure of ozone in regions with complex water-land boundaries. Preliminary comparison results will be presented on ozone temporal and vertical differences between NAQFC and the TOLNet lidars along with example case studies to illustrate insights into boundary layer and surface processes of trace gases.

Timothy Berkoff↗
NASA NTRS2022

The Ozone–Climate Penalty Over South America and Africa By 2100

Climate change has the potential to increase surface ozone (O3) concentrations, known as the “ozone–climate penalty”, through changes to atmospheric chemistry, transport and dry deposition. In the tropics, the response of surface O3 to changing climate is relatively understudied but has important consequences for air pollution and human and ecosystem health. In this study, we evaluate the change in surface O3 due to climate change over South America and Africa using three state-of-the-art Earth system models that follow the Shared Socioeconomic Pathway 3-7.0 emission scenario from CMIP6. In order to quantify changes due to climate change alone, we evaluate the difference between simulations including climate change and simulations with a fixed present-day climate. We find that by 2100, models predict an ozone–climate penalty in areas where O3 is already predicted to be high due to the impacts of precursor emissions, namely urban and biomass burning areas, although on average, models predict a decrease in surface O3 due to climate change. We identify a small but robust positive trend in annual mean surface O3 over polluted areas. Additionally, during biomass burning seasons, seasonal mean O3 concentrations increase by 15 ppb (model range 12 to 18 ppb) in areas with substantial biomass burning such as the arc of deforestation in the Amazon. The ozone–climate penalty in polluted areas is shown to be driven by an increased rate of O3 chemical production, which is strongly influenced by NOx concentrations and is therefore specific to the emission pathway chosen. Multiple linear regression finds the change in NOx concentration to be a strong predictor of the change in O3 production, whereas increased isoprene emission rate is positively correlated with increased O3 destruction, suggesting NOx-limited conditions over the majority of tropical Africa and South America. However, models disagree on the role of climate change in remote, low-NOx regions, partly because of significant differences in NOx concentrations produced by each model. We also find that the magnitude and location of the ozone–climate penalty in the Congo Basin has greater inter-model variation than that in the Amazon, so further model development and validation are needed to constrain the response in central Africa. We conclude that if the climate were to change according to the emission scenario used here, models predict that forested areas in biomass burning locations and urban populations will be at increasing risk of high O3 exposure, irrespective of any direct impacts on O3 via the prescribed emission scenario.

Surface ozone↗
NASA NTRS2000

Lidar Remote Sensing for Industry and Environment Monitoring

Contents include the following: 1. Keynote paper: Overview of lidar technology for industrial and environmental monitoring in Japan. 2. lidar technology I: NASA's future active remote sensing mission for earth science. Geometrical detector consideration s in laser sensing application (invited paper). 3. Lidar technology II: High-power femtosecond light strings as novel atmospheric probes (invited paper). Design of a compact high-sensitivity aerosol profiling lidar. 4. Lasers for lidars: High-energy 2 microns laser for multiple lidar applications. New submount requirement of conductively cooled laser diodes for lidar applications. 5. Tropospheric aerosols and clouds I: Lidar monitoring of clouds and aerosols at the facility for atmospheric remote sensing (invited paper). Measurement of asian dust by using multiwavelength lidar. Global monitoring of clouds and aerosols using a network of micropulse lidar systems. 6. Troposphere aerosols and clouds II: Scanning lidar measurements of marine aerosol fields at a coastal site in Hawaii. 7. Tropospheric aerosols and clouds III: Formation of ice cloud from asian dust particles in the upper troposphere. Atmospheric boundary layer observation by ground-based lidar at KMITL, Thailand (13 deg N, 100 deg. E). 8. Boundary layer, urban pollution: Studies of the spatial correlation between urban aerosols and local traffic congestion using a slant angle scanning on the research vessel Mirai. 9. Middle atmosphere: Lidar-observed arctic PSC's over Svalbard (invited paper). Sodium temperature lidar measurements of the mesopause region over Syowa Station. 10. Differential absorption lidar (dIAL) and DOAS: Airborne UV DIAL measurements of ozone and aerosols (invited paper). Measurement of water vapor, surface ozone, and ethylene using differential absorption lidar. 12. Space lidar I: Lightweight lidar telescopes for space applications (invited paper). Coherent lidar development for Doppler wind measurement from the International Space Station. 13. Space lidar II: Using coherent Doppler lidar to estimate river discharge. 14. Poster session: Lidar technology, optics for lidar. Laser for lidar. Middle atmosphere observations. Tropospheric observations (aerosols, clouds). Boundary layer, urban pollution. Differential absorption lidar. Doppler lidar. and Space lidar.

Singh, Upendra N.↗
NASA NTRS2002

Urban and Rural Ozone Collect over Lusaka (Zambia, 15.5 S, 28 E) during SAFARI-2000 (September 2000)

In early September, throughout south central Africa, seasonal clearing of dry vegetation and the production of charcoal for cooking leads to intense smoke haze and ozone formation. Ozone soundings made over Lusaka in early September 2000 recorded layers of high ozone (greater than 125 ppbv at 5 km) during two stagnant periods, broken by a frontal passage that reduced boundary layer ozone by 30%. During the 6-day measurement period, surface ozone concentrations ranged from 50-95 ppbv and integrated tropospheric ozone from the soundings was 39-54 Dobson Units (note 1.3 km elevation at the launch site). A stable layer of high ozone at 2-5 km was advected from rural burning regions in western Zambia and neighboring countries, making Lusaka a collection point for transboundary pollution. This is confirmed by trajectories that show ozone leaving Angola, Namibia, Botswana and South Africa before heading toward the Indian Ocean and returning to Lusaka via Mozambique and Zimbabwe. Ozone in the mixed layer at Lusaka is heavily influenced by local sources.

Thompson, Anne M.↗
NASA NTRS2001

Urban and Rural Ozone Pollution Over Lusaka (Zambia, 15.5S, 25E) During SAFARI-2000 (September 2000)

In early September, throughout south central Africa, seasonal clearing of dry vegetation and the production of charcoal for cooking leads to intense smoke haze and ozone formation. Ozone soundings made over Lusaka during a six-day period in early September 2000 recorded layers of high ozone (greater than 125 ppbv at 5 km) during two stagnant periods, interspersed by a frontal passage that reduced boundary layer ozone by 30 percent. Smoke aerosol column variations aloft and total ozone were monitored by a sun photometer. During the 6-day measurement period, surface ozone concentrations ranged from 50-95 ppbv and integrated tropospheric ozone from the soundings was 39- 54 Dobson Units (note 1.3 km elevation at the launch site). High ozone concentrations above the mixed and inversion layers were advected from rural burning regions in western Zambia where SAFARI aircraft and ground-based instruments observed intense biomass fires and elevated aerosol and trace gas amounts. TOMS tropospheric ozone and smoke aerosols products show the distribution of biomass burning and associated pollution throughout southern Africa in September 2000. Animations of satellite images and trajectories confirm pollutant recirculation over south central African fires, exit of ozone from Mozambique and Tanzania to the Indian Ocean and the characteristic buildup of tropospheric ozone over the Atlantic from western African outflow.

Thompson, Anne M.↗
NASA NTRS2016

Lightning NOx and Impacts on Air Quality

Lightning generates relatively large but uncertain quantities of nitrogen oxides, critical precursors for ozone and hydroxyl radical (OH), the primary tropospheric oxidants. Lightning nitrogen oxide strongly influences background ozone and OH due to high ozone production efficiencies in the free troposphere, effecting small but non-negligible contributions to surface pollutant concentrations. Lightning globally contributes 3-4 ppbv of simulated annual-mean policy-relevant background (PRB) surface ozone, comprised of local, regional, and hemispheric components, and up to 18 ppbv during individual events. Feedbacks via methane may counter some of these effects on decadal time scales. Lightning contributes approximately 1 percent to annual-mean surface particulate matter, as a direct precursor and by promoting faster oxidation of other precursors. Lightning also ignites wildfires and contributes to nitrogen deposition. Urban pollution influences lightning itself, with implications for regional lightning-nitrogen oxide production and feedbacks on downwind surface pollution. How lightning emissions will change in a warming world remains uncertain.

Reactive nitrogen oxides↗
NASA NTRS2022

Multidecadal Trends in Ozone Chemistry in the Baltimore-Washington Region

Over the past four decades, policy-led reductions in anthropogenic emissions have improved air quality over the Baltimore-Washington region (BWR). Most of the improvements in meeting the ozone air quality metrics (NAAQS) did not occur until the early 2000s despite large reductions in ozone precursors (NOx, CO, and volatile organic compounds (VOCs)) in the prior decades. We use observations of ozone and ozone precursors from satellites, ground-based sites, and the 2011 DISCOVER-AQ aircraft campaign in Maryland to illustrate how ozone chemistry in the BWR evolved between 1972 and 2019. Analysis of weekday vs weekend probability of ozone exceedance indicates the BWR transitioned to the NOx-limited regime by 2000–2003. A data-constrained box model agrees with this transition period and illustrates the key roles of reduced emissions of formaldehyde (HCHO), aromatics, and other VOCs since 1996, which reduced the peak of ozone production at the time of the transition and likely prevented the BWR from experiencing worsening surface air quality as the region transitioned to NOx-limited chemistry. Analysis of satellite observations of tropospheric column HCHO to NO2 analyzed using a new approach for evaluation of chemical regimes derived from DISCOVER-AQ data also provide a consistent depiction of the timing of the transition period that we infer from ground-based observations and the box model. Finally, despite significant improvements in air quality over the past two decades, the BWR still has not met the EPA standard for surface ozone. With predominantly NOx-limited ozone chemistry over the BWR, continued decreases in emission of NOx will slow the rate of ozone production and help improve air quality. We highlight emissions of NO2 from the diesel truck fleet as a worthwhile focus for future policy because emissions from this source appear to influence day-of-week variations in observed NO2, with an accompanying effect on ozone.

Ozone↗
NASA NTRS1995

Ozone, Tropospheric

In the early part of the 20th century, ground-based and balloon-borne measurements discovered that most of atmosphere's ozone is located in the stratosphere with highest concentrations located between 15 and 30 km (9,3 and 18.6 miles). For a long time, it was believed that tropospheric ozone originated from the stratosphere and that most of it was destroyed by contact with the earth's surface. Ozone, O3, was known to be produced by the photo-dissociation of molecular oxygen, O2, a process that can only occur at wavelengths shorter than 242 nm. Because such short-wave-length radiation is present only in the stratosphere, no tropospheric ozone production is possible by this mechanism. In the 1940s, however, it became obvious that production of ozone was also taking place in the troposphere. The overall reaction mechanism was eventually identified by Arie Haagen-Smit of the California Institute of Technology, in highly polluted southern California. The copious emissions from the numerous cars driven there as a result of the mass migration to Los Angeles after World War 2 created the new unpleasant phenomenon of photochemical smog, the primary component of which is ozone. These high levels of ozone were injuring vegetable crops, causing women's nylons to run, and generating increasing respiratory and eye-irritation problems for the populace. Our knowledge of tropospheric ozone increased dramatically in the early 1950s as monitoring stations and search centers were established throughout southern California to see what could be done to combat this threat to human health and the environment.

Fishman, Jack↗
NASA NTRS1993

Dynamical response of the tropical total ozone to sea surface temperature changes

Interannual variations of total ozone in the equatorial region are discussed in terms of the lower-stratospheric dynamical processes associated with sea surface temperature (SST) changes on an El Nino-Southern Oscillation time scale. Tropospheric diabatic heating by the latent heat release in convective systems drives the interannual variations of tropopause height and atmospheric vertical motions. The adiabatic cooling associated with the dynamically forced ascending motion is subject to radiative heating, which further extends the upwelling motion into the stratosphere. SST variations can thus influence total ozone amounts by changing the tropopause height and vertical advection through modulation of tropospheric diabatic heating. Mechanistic relationships that describe total ozone fluctuations through the advection effect and the tropopause effect of SST variations are derived using the equivalent potential temperature. Total ozone fluctuations are estimated using a quantitative formulation of these mechanistic equations together with the observed SST data. These results indicate that the interannual variations of the zonal wave component of equatorial total ozone are governed by the tropopause effect of SST variations. Preliminary investigation suggests that the annual cycle of tropical total ozone is coupled to the tropopause height changes under the influence of the planetary wave-induced lower-stratospheric temperature rather than local SST.

Hasebe, Fumio↗
NASA NTRS2015

Impact of Transpacific Aerosol on Air Quality over the United States: A Perspective from Aerosol-Cloud-Radiation Interactions

Observations have well established that aerosols from various sources in Asia, Europe, and Africa can travel across the Pacific and reach the contiguous United States (U.S.) at least on episodic bases throughout a year, with a maximum import in spring. The imported aerosol not only can serve as an additional source to regional air pollution (e.g., direct input), but also can influence regional air quality through the aerosol-cloud-radiation (ACR) interactions that change local and regional meteorology. This study assessed impacts of the transpacific aerosol on air quality, focusing on surface ozone and PM2.5, over the U.S. using the NASA Unified Weather Research Forecast model. Based on the results of 3- month (April to June of 2010) simulations, the impact of direct input (as an additional source) of transpacific aerosol caused an increase of surface PM2.5 concentration by approximately 1.5 micro-g/cu m over the west coast and about 0.5 micro-g/cu m over the east coast of the U.S. By influencing key meteorological processes through the ACR interactions, the transpacific aerosol exerted a significant effect on both surface PM2.5 (+/-6 micro-g/cu m3) and ozone (+/-12 ppbv) over the central and eastern U.S. This suggests that the transpacific transport of aerosol could either improve or deteriorate local air quality and complicate local effort toward the compliance with the U.S. National Ambient Air Quality Standards.

Tao, Zhining↗
NASA NTRS2008

The Influence of European Pollution on Ozone in the Near East and Northern Africa

We present a modeling study of the long-range transport of pollution from Europe, showing that European emissions regularly elevate surface ozone by as much as 20 ppbv in summer in northern Africa and the Near East. European emissions cause 50-150 additional violations per year (i.e. above those that would occur without European pollution) of the European health standard for ozone (8-h average greater than 120 micrograms per cubic meters or approximately 60 ppbv) in northern Africa and the Near East. We estimate that European ozone pollution is responsible for 50 000 premature mortalities globally each year, of which the majority occurs outside of Europe itself, including 37% (19 000) in northern Africa and the Near East. Much of the pollution from Europe is exported southward at low altitudes in summer to the Mediterranean Sea, northern Africa and the Near East, regions with favorable photochemical environments for ozone production. Our results suggest that assessments of the human health benefits of reducing ozone precursor emissions in Europe should include effects outside of Europe, and that comprehensive planning to improve air quality in northern Africa and the Near East likely needs to address European emissions.

Duncan, B. N.↗