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NASA NTRS2000

Elevated Tropospheric Ozone Over the South Tropical Atlantic in January-February 1999: An Ozone Paradox Due to Interhemispheric Transport, Lightning, or Stratospheric Exchange?

On this first North American to southern African oceanographic cruise with ozonesonde launches (January and February 1999 on board the NOAA Research Vessel Ronald H Brown between Norfolk, VA, and Cape Town, South Africa) we found: (1) high ozone, CO, and aerosols off northern equatorial Africa from biomass burning, but even higher ozone concentrations off southern Africa which was not burning - an "ozone paradox"; (2) TOMS satellite evidence that south Atlantic elevated ozone in January-February 1999 was a regional feature similar in extent to the well-known September-October ozone maximum. Several mechanisms are considered to explain the "ozone paradox." Convection transporting air from the lower troposphere rich in ozone and/or ozone precursors to the upper troposphere through the ITCZ (intertropical Convergence Zone) may lead to cross-hemisphere transport of pollution. This is supported by trajectory linkage of lower-tropospheric ozone maxima with smoke seen by the TOMS satellite. Lightning-generated NO (nitric oxide) leading to ozone peaks of > 100 ppbv observed at 7-10 km altitude is another explanation. The TRMM (Tropical Rainfall Measuring Mission) Lightning Imaging Sounder shows many lightning flashes over southern Africa, which trajectories link to the high-ozone layers south of the ITCZ. The highest ozone peaks in the middle troposphere correspond to very low water vapor, which may point to photochemical destruction of ozone or subsidence from the upper troposphere which had interacted with stratospheric ozone.

Thompson, Anne M.↗
NASA NTRS1998

A TOMS-Based View of Tropical Tropospheric Ozone (OTTO) From Large Fires Associated with the 1997-1998 El Nino

Since the launch of Earth-Probe TOMS in July 1 996, we have been producing tropical tropospheric ozone (TTO) maps (10S - 10N), in gridded format, l x 2 degrees, in near-real time. These images, along with images from the full ADEOS-TOMS record of TTO (Sept. 1996 - May 1997) can be viewed on a homepage: http://metosrv2.umd,edu/-tropo). The TTO maps, based on the modified-residual method of Hudson and Thompson [1998], have been validated using ozonesondes from Ascension (8S, 15W), Nairobi (2S, 36E) and American Samoa (14S, 171W). The fires associated with El Nino-induced dryness are exhibited regionally as high tropospheric ozone column (> 60 Dobson Units) with high absorbing aerosol (smoke) signal in TOMS [J. R. Herman, personal communication, 1998]. Episodes of high TTO in 1997-98 will be shown. Regional TTO over Indonesia during the 1997-98 period will be highlighted and comparisons will be made with TTO in that region taken from the 1979-92 Nimbus/TOMS TTO record.

Thompson, Anne M.↗
NASA NTRSDate not supplied

Tropical Tropospheric Ozone Trends (1990 to 2022): A Re-evaluation Based on SHADOZ and IAGOS Profiles and TOMS/OMI Columns

Changes in tropical tropospheric ozone (TTO) are of importance because this region spans roughly a third of the Earth and portions of it are experiencing variability in trends of ozone precursors (CO, NO x , CH 4 and nonmethane hydrocarbons) associated with economic growth and fires. In addition to ozone changes affecting radiative forcing, tropical ozone is an important source of the OH radical and thus, the oxidizing capacity of the planet (Thompson, 1992). Recent studies examining TTO trends satellite and in-situ observations over the past ~25 years include: Thompson et al., JGR, 2021; Gaudel et al., ACP, 2023; Stauffer et al., ACP, 2023. The results show considerable regional and seasonal variability in TTO trends and sensitivity to data selection, frequency, and statistical method used. The satellite data vary most widely in method, time period and reliability. Here we revisit trends for the 1990-2022 period with the best-characterized buv-based satellite products that span that period (derived from TOMS and OMI, Ziemke et al., 2019). The satellite-based trends are compared to trends based on in-situ data from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network (1998-2022), measurements from selected pre-SHADOZ and IAGOS commercial aircraft data (Gaudel et al., 2023). Among sensitivities examined are the dependence of ozone trends on start and end years, impacts of ENSO events and the COVID-19 perturbation to emissions. Two statistical methods are used, quantile regression (QR) and multiple linear regression (MLR). Trends of total TTO, ozone segments in the boundary layer (to ~700 hPa), and free troposphere (700-300 hPa) are compared.

ozone, OMI, tropospheric ozone, SHADOZ↗
NASA NTRS2021

COVID-19 Crisis Reduces Free Tropospheric Ozone Across the Northern Hemisphere

Throughout spring and summer 2020, ozone stations in the northern extratropics recorded unusually low ozone in the free troposphere. From April to August, and from 1 to 8 kilometers altitude, ozone was on average 7% (≈4 nmol/mol) below the 2000–2020 climatological mean. Such low ozone, over several months, and at so many stations, has not been observed in any previous year since at least 2000. Atmospheric composition analyses from the Copernicus Atmosphere Monitoring Service and simulations from the NASA GMI model indicate that the large 2020 springtime ozone depletion in the Arctic stratosphere contributed less than one-quarter of the observed tropospheric anomaly. The observed anomaly is consistent with recent chemistry-climate model simulations, which assume emissions reductions similar to those caused by the COVID-19 crisis. COVID-19 related emissions reductions appear to be the major cause for the observed reduced free tropospheric ozone in 2020.

COVID-19↗
NASA NTRS2000

Model Study of the Sources of Upper Tropospheric Ozone Over The Atlantic, with Emphasis on Interhemispheric Asymmetries

Measurements of ozone and aerosols from ships transecting the Atlantic Ocean reveal considerable interhemispheric asymmetries in the vertical structure of the ozone distribution. There is much more upper tropospheric ozone to the South of the Equator than in the northern hemisphere. These profiles suggest that the air in the southern hemispheric tropics and subtropics has a source in the stratosphere, while that in the northern hemisphere originates in the boundary layer. A model experiment designed to investigate this problem will be discussed. They are based on a new general circulation model, based on a Finite-Volume dynamical core and the physical parametrizations from the Community Climate Model at the National Center for Atmospheric Research (NCAR). The model simulates a climatological state in reasonable agreement with observations, comparable to other contemporary climate models, but has a much more accurate transport capability than most other present-day models. The experiment involves using a suite of tracers, designed to highlight air from different source regions. Some of these (water vapor and ozone) represent real atmospheric quantities, while others are markers which indicate whether the air originates in the stratosphere, the boundary layer, or has traversed regions of convection (for example). The experiments were run for periods of up to one month, initialized from snapshots from a long climate integration of the model. A sample of results will be presented, chosen to illustrate the different sources of air in the upper troposphere and the physical mechanisms by which these air parcels arrived there.

Pawson, Steven↗
NASA NTRS1978

Tropospheric ozone distributions measured with an airborne laser absorption spectrometer

Measurements of tropospheric ozone have been made in the southern and middle California regions and over the Pacific Ocean during two series of flights in February and May 1977. The data were obtained by using a laser absorption spectrometer, a nadir-viewing instrument which remotely measures the ozone column abundance between ground level and aircraft altitude by interacting with ozone at specific wavelengths near 9.5 microns. The measurements indicate significantly lower ozone abundances above the Mojave Desert region as compared with farm, forest, and urban areas. The average tropospheric column density was found to be 0.0027 atm cm/km over the California region and 0.0035 atm cm/km over the Pacific Ocean region 1000-2000 km west of the coast of Mexico.

Menzies, R. T.↗
NASA NTRS1998

Effects of 1997-1998 El Nino on Tropospheric Ozone and Water Vapor

This paper analyzes the impact of the 1997-1998 El Nino on tropospheric column ozone and tropospheric water vapor derived respectively from the Total Ozone Mapping Spectrometer (TOMS) on Earth Probe and the Microwave Limb Scanning instrument on the Upper Atmosphere Research Satellite. The 1997-1998 El Nino, characterized by an anomalous increase in sea-surface temperature (SST) across the eastern and central tropical Pacific Ocean, is one of the strongest El Nino Southern Oscillation (ENSO) events of the century, comparable in magnitude to the 1982-1983 episode. The major impact of the SST change has been the shift in the convection pattern from the western to the eastern Pacific affecting the response of rain-producing cumulonimbus. As a result, there has been a significant increase in rainfall over the eastern Pacific and a decrease over the western Pacific and Indonesia. The dryness in the Indonesian region has contributed to large-scale burning by uncontrolled wildfires in the tropical rainforests of Sumatra and Borneo. Our study shows that tropospheric column ozone decreased by 4-8 Dobson units (DU) in the eastern Pacific and increased by about 10-20 DU in the western Pacific largely as a result of the eastward shift of the tropical convective activity as inferred from National Oceanic and Atmospheric Administration (NOAA) outgoing longwave radiation (OLR) data. The effect of this shift is also evident in the upper tropospheric water vapor mixing ratio which varies inversely as ozone (O3). These conclusions are qualitatively consistent with the changes in atmospheric circulation derived from zonal and vertical wind data obtained from the Goddard Earth Observing System data assimilation analyses. The changes in tropospheric column O3 during the course of the 1997-1998 El Nino appear to be caused by a combination of large-scale circulation processes associated with the shift in the tropical convection pattern and surface/boundary layer processes associated with forest fires in the Indonesian region.

Chandra, S.↗
NASA NTRS2008

Global Radiative Forcing of Coupled Tropospheric Ozone and Aerosols in a Unified General Circulation Model

Global simulations of sea salt and mineral dust aerosols are integrated into a previously developed unified general circulation model (GCM), the Goddard Institute for Space Studies (GISS) GCM II', that simulates coupled tropospheric ozone-NOx-hydrocarbon chemistry and sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon aerosols. The fully coupled gas-aerosol unified GCM allows one to evaluate the extent to which global burdens, radiative forcing, and eventually climate feedbacks of ozone and aerosols are influenced by gas-aerosol chemical interactions. Estimated present-day global burdens of sea salt and mineral dust are 6.93 and 18.1 Tg with lifetimes of 0.4 and 3.9 days, respectively. The GCM is applied to estimate current top of atmosphere (TOA) and surface radiative forcing by tropospheric ozone and all natural and anthropogenic aerosol components. The global annual mean value of the radiative forcing by tropospheric ozone is estimated to be +0.53 W m(sup -2) at TOA and +0.07 W m(sup -2) at the Earth's surface. Global, annual average TOA and surface radiative forcing by all aerosols are estimated as -0.72 and -4.04 W m(sup -2), respectively. While the predicted highest aerosol cooling and heating at TOA are -10 and +12 W m(sup -2) respectively, surface forcing can reach values as high as -30 W m(sup -2), mainly caused by the absorption by black carbon, mineral dust, and OC. We also estimate the effects of chemistry-aerosol coupling on forcing estimates based on currently available understanding of heterogeneous reactions on aerosols. Through altering the burdens of sulfate, nitrate, and ozone, heterogeneous reactions are predicted to change the global mean TOA forcing of aerosols by 17% and influence global mean TOA forcing of tropospheric ozone by 15%.

Liao, Hong↗
NASA NTRS2010

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↗
NASA NTRS1977

Photochemistry of tropospheric ozone

A photochemical equilibrium model of minor constituent chemistry in the troposphere was constructed to investigate the photochemistry of tropospheric ozone. We find that photochemical production must be supplemented by additional sources to account for observed ozone levels in clean air, while photochemical loss is more important than surface destruction as an ozone loss mechanism. Photochemically produced ozone is sensitive to the NO(x) background in the model, exhibiting a maximum of about 0.5 ppb of NO(x).

Stewart, R. W.↗
NASA NTRS2000

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.↗
NASA NTRS1994

Tropospheric ozone in the western Pacific Rim: Analysis of satellite and surface-based observations along with comprehensive 3-D model simulations

Tropospheric ozone production and transport in mid-latitude eastern Asia is studied. Data analysis of surface-based ozone measurements in Japan and satellite-based tropospheric column measurements of the entire western Pacific Rim are combined with results from three-dimensional model simulations to investigate the diurnal, seasonal and long-term variations of ozone in this region. Surface ozone measurements from Japan show distinct seasonal variation with a spring peak and summer minimum. Satellite studies of the entire tropospheric column of ozone show high concentrations in both the spring and summer seasons. Finally, preliminary model simulation studies show good agreement with observed values.

Young, Sun-Woo↗
NASA NTRS2020

Sensitivity of Tropospheric Ozone Over the Southeast USA to Dry Deposition

Dry deposition (DD) is a major loss process for tropospheric ozone and some reactive nitrogen and carbon precursors. We investigate the response of summertime ozone and its production chemistry over the Southeast United States (USA) to variability in this sink. Turning off DD of oxidized nitrogen, ozone, or all species over the United States in the Geophysical Fluid Dynamics Laboratory AM3 model increases regional mean surface ozone by 5, 18, or 25 ppb, respectively. Additional sensitivity simulations demonstrate that, assuming linearity, surface ozone has a similar sensitivity to ozone DD as to NOx emissions. Trends in ozone production efficiency derived from observed relationships between ozone and precursor oxidation products may not solely reflect precursor emission changes if ozone DD varies (e.g., with meteorology). We conclude that DD variability merits consideration when interpreting observed ozone trends. Quantifying the impact of changes in sinks versus sources will require long‐term DD measurements across the region of interest.

dry deposition↗
NASA NTRS2011

The Response of Tropical Tropospheric Ozone to ENSO

We have successfully reproduced the Ozone ENSO Index (OEI) in the Goddard Earth Observing System (GEOS) chemistry-climate model (CCM) forced by observed sea surface temperatures over a 25-year period. The vertical ozone response to ENSO is consistent with changes in the Walker circulation. We derive the sensitivity of simulated ozone to ENSO variations using linear regression analysis. The western Pacific and Indian Ocean region shows similar positive ozone sensitivities from the surface to the upper troposphere, in response to positive anomalies in the Nino 3.4 Index. The eastern and central Pacific region shows negative sensitivities with the largest sensitivity in the upper troposphere. This vertical response compares well with that derived from SHADOZ ozonesondes in each region. The OEI reveals a response of tropospheric ozone to circulation change that is nearly independent of changes in emissions and thus it is potentially useful in chemistry-climate model evaluation.

Oman, L. D.↗
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 NTRS2016

Western US Tropospheric Ozone: An Assessment of Vertical and Seasonal Variations over California and Nevada

In the rural western US free-tropospheric O3 has risen in recent years as a result of rising Asian emissions, deep stratospheric intrusions and more frequent wildfires. This increasing O3 trend combined with the high surface elevation of much of the western US, which aids mixing between boundary layer and free-troposphere, pose challenges in attaining the more stringent O3 National Ambient Air Quality Standard (NAAQS) at many western US rural surface sites. As such, the ability to identify various sources and transport mechanisms that contribute towards surface O3 is increasingly important. This paper analyzes vertical profiles of O3 from the Alpha Jet Atmospheric eXperiment (AJAX) over California and Nevada, ozonesondes from Trinidad Head, CA and tropospheric ozone profiles from the differential absorption lidar (DIAL) at the JPL Table Mountain Facility, CA. Surface O3 from the US EPA Clean air Status and Trends Network (CASNET) are used to discuss surface trends. GEOS-Chem determines the trends in regional O3 and assess the contributions of various sources on surface O3. And Realtime Air Quality Modeling System (RAQMS) is used to forecast and interpret free-tropospheric observations. Specifically we will address the following questions: What are the effects of the lowered NAAQS? Do we observe elevated O3 during 2012 at surface sites reported in previous studies? And if so, what are the causes? How variable is free-tropospheric O3 over California and Nevada? How frequently do we observe high O3 lamina in the free troposphere and what are the surface impacts?

tropospheric↗
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↗