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All sourcesNASA NTRSDOE OSTI
NASA NTRS2002

Insights into Tropical Tropospheric Ozone from the SHADOZ Network

The first view of lower stratospheric and upper tropospheric structure from sondes is provided by a 3-year, 10-site record from the Southern Hemisphere ADditional OZonesondes (SHADOZ) network: http://code9 16.gsfc.nasa.gov/Data_services/shadoz. Observations covering 1998-2000 were made over Ascension Island; Nairobi, Kenya; Irene, South Africa; La Reunion Island; Watukosek, Java; Fiji; Tahiti; American Samoa; San Cristobal, Galapagos; Natal, Brazil. Taking the UT/LS (upper troposphere-lower stratosphere) as the region between 12 and 17 km, we examine ozone variability in this region on a week-to- week and seasonal basis. The tropopause is lower in September-October-November than in March-April-May, when ozone is a minimum at most SHADOZ stations. A zonal wave-one pattern (referring to ozone mixing ratios greater over the Atlantic and adjacent continents than over the Pacific and eastern Indian Ocean), persists all year. The wave, predominantly in the troposphere and with variable magnitude, appears to be due to general circulation - with subsidence over the Atlantic and frequent deep convection over the Pacific and Indian Ocean. The variability of deep convection - most prominent at Java, Fiji, Samoa and Natal - is explored in time-vs-altitude ozone curtains. Stratospheric incursions into the troposphere are most prominent in soundings at Irene and Reunion Island.

Thompson, A. M.↗
NASA NTRS1992

First Results from TROLIX 1991: an Intercomparison of Tropospheric Ozone Lidars

Within the framework of the European environmental research programme EUROTRAC, lidar systems for routine measurements of vertical ozone profiles throughout the planetary boundary layer and the free troposphere are currently under development. Several of these systems are now operational and an intercomparison experiment was undertaken in the period from June 10 to June 28, 1991 in Bilthoven, the Netherlands. The main scientific objectives defined for the campaign are: (1) compare the lidar measurements to in situ measurements of the ozone concentration; (2) determine how many and which wavelengths are needed for a sufficiently accurate ozone retrieval in the lower troposphere under realistic conditions; (3) assess the accuracy that can be achieved under realistic conditions; and (4) compare the performance of the participating systems.

Apituley, A.↗
NASA NTRS1984

Measurements of free tropospheric ozone - An aircraft survey from 44 degrees north to 46 south latitude

Ozone data were obtained in the free troposphere at altitudes of 5 to 7.5 km and at latitudes from 44 degrees N to 46 degrees S during a 3-week period from October 19 to November 4, 1982. Flight trajectories included the continental U.S., Central America, and the western coast of South America. Maximum observed ozone was 110 ppb at about 41 degrees S latitude and at an altitude of 7.3 km (msl). Analysis of the data as a function of latitude showed a region of elevated ozone in the southern latitudes extending from about 2 degrees to 30 degrees in which latitudinal ozone averages (2 degree bands) peaked at about 80 ppb. Ozone concentrations, measured at northern latitudes, were lower, averaging about 35 ppb. A discussion of the data, including comparison with other ozone data sets, is presented.

Gregory, G. L.↗
NASA NTRS1994

Enhancement of free tropospheric ozone production by deep convection

It is found from model simulations of trace gas and meteorological data from aircraft campaigns that deep convection may enhance the potential for photochemical ozone production in the middle and upper troposphere by up to a factor of 60. Examination of half a dozen individual convective episodes show that the degree of enhancement is highly variable. Factors affecting enhancement include boundary layer NO(x) mixing ratios, differences in the strength and structure of convective cells, as well as variation in the amount of background pollution already in the free troposphere.

Pickering, Kenneth E.↗
NASA NTRS1990

Model calculations of tropospheric ozone production potential following observed convective events

The profiles of CO, NO, O3, water vapor, and temperature, observed in 1985 during and after a series of convective events over rural areas of the south-central United States, were used to model the nonurban ozone production rates and to evaluate the effects of convective clouds on the tropospheric trace-gas chemistry. A comparison of trace-gas profiles measured in and around a large cumulonimbus during its dissipation showed that ozone production in the upper troposphere may be increased fourfold by convection relative to undisturbed air. The convective enhancement of O3 production for the entire tropospheric comlumn was found to be about 50 percent.

Pickering, Kenneth E.↗
NASA NTRS1988

Tropospheric ozone and aerosol distributions across the Amazon Basin

As a part of the NASA Global Tropospheric Experiment to study the Amazon boundary layer, ozone and aerosol distributions were made measured in July-August 1985 by a NASA Electra aircraft on several long-range flights spanning different areas between Tabatinga and Belem, Brazil. Both positive and negative correlations were found in PBL between aerosol concentrations and O3 mixing ratios. The negative correlations result from the downward transport of relatively clean O3-rich air from the upper troposphere into PBL (which normally has higher aerosol loading and lower O3 concentrations than troposphere); positive correlations are found in biomass-burning plumes, where the aerosols are emitted into the air and O3 is photochemically produced. It was found that, in the dry season, a significant portion of the ozone over the rain forest is a result of biomass burning and that the distribution of photochemically produced O3 is strongly affected by synoptic-scale transport from large fires to the south/southeast.

Browell, E. V.↗
NASA NTRS1992

Free tropospheric ozone production following entrainment of urban plumes into deep convection

It is shown that rapid vertical transport of air from urban plumes through deep convective clouds can cause substantial enhancement of the rate of O3 production in the free troposphere. Simulation of convective redistribution and subsequent photochemistry of an urban plume from Oklahoma City during the 1985 PRESTORM campaign shows enhancement of O3 production in the free tropospheric cloud outflow layer by a factor of almost 4. In contrast, simulation of convective transport of an urban plume from Manaus, Brazil, into a prestine free troposphere during GTE/ABLE 2B (1987), followed by a photochemical simulation, showed enhancement of O3 production by a factor of 35. The reasons for the different enhancements are (1) intensity of cloud vertical motion; (2) initial boundary layer O3 precursor concentrations; and (3) initial amount of background free tropospheric NO(x). Convective transport of ozone precursors to the middle and upper troposphere allows the resulting O3 to spread over large geographic regions, rather than being confined to the lower troposphere where loss processes are much more rapid. Conversely, as air with lower NO descends and replaces more polluted air, there is greater O3 production efficiency per molecule of NO in the boundary layer following convective transport. As a result, over 30 percent more ozone could be produced in the entire tropospheric column in the first 24 hours following convective transport of urban plumes.

Pickering, Kenneth E.↗
NASA NTRS2012

The Role of Lightning in Controlling Interannual Variability of Tropical Tropospheric Ozone and OH and its Implications for Climate

Nitrogen oxides (NO(x) = NO + NO2) produced by lightning make a major contribution to the production of the dominant tropospheric oxidants (OH and ozone). These oxidants control the lifetime of many trace gases including long-lived greenhouse gases, and control the source-receptor relationship of inter-hemispheric pollutant transport. Lightning is affected by meteorological variability, and therefore represents a potentially important tropospheric chemistry-climate feedback. Understanding how interannual variability (IAV) in lightning affects IAV in ozone and OH in the recent past is important if we are to predict how oxidant levels may change in a future warmer climate. However, lightning parameterizations for chemical transport models (CTMs) show low skill in reproducing even climatological distributions of flash rates from the Lightning Imaging Sensor (LIS) and the Optical Transient Detector (OTD) satellite instruments. We present an optimized regional scaling algorithm for CTMs that enables sufficient sampling of spatiotemporally sparse satellite lightning data from LIS to constrain the spatial, seasonal, and interannual variability of tropical lightning. We construct a monthly time series of lightning flash rates for 1998-2010 and 35degS-35degN, and find a correlation of IAV in total tropical lightning with El Nino. We use the IAV-constraint to drive a 9-year hindcast (1998-2006) of the GEOS-Chem 3D chemical transport model, and find the increased IAV in LNO(x) drives increased IAV in ozone and OH, improving the model fs ability to simulate both. Although lightning contributes more than any other emission source to IAV in ozone, we find ozone more sensitive to meteorology, particularly convective transport. However, we find IAV in OH to be highly sensitive to lightning NO(x), and the constraint improves the ability of the model to capture the temporal behavior of OH anomalies inferred from observations of methyl chloroform and other gases. The sensitivity of OH is explained using photochemical reaction rates which show a "magnification" effect of the initial lightning NO perturbation on OH primary production, HO(x) recycling, and OH loss frequencies. This influence on OH may represent a negative feedback, if lightning increases in a warming world..

Murray, Lee T.↗
NASA NTRS2007

Mechanisms for the Intraseasonal Variability of Tropospheric Ozone over the Indian Ocean during the Winter Monsoon

We synthesize daily sonde (vertical) information and daily satellite (horizontal) information to provide an empirical description of ozone origins over the northern Indian Ocean during the INDOEX (Indian Ocean Experiment) field campaign (February-March 1999). This area is shown to be a significant portion of the "high-ozone tropics". East-west O3 features and their flow are identified, and ozone origins are compared to other tropical regions, using water vapor as a second tracer. In the study period, multiple processes contribute to O3 column enhancements, their importance varying strongly by latitude: (1) Low-altitude O3 pollution over the northern Indian Ocean mainly originates from the Indian subcontinent and is traceable to high emission areas. Convective activity south of Sri Lanka helps direct ozone outflow from the northern Indian subcontinent. (2) Middle tropospheric O3 maxima over the northern Indian Ocean originate from various sources, often transitioning within a few hours. Convective venting of Asian pollutants can add 20-30 ppbv to the middle troposphere at 5degN-10degN, alternating with stratospheric influence. (3) A number of cases suggest that strong mixing-in of stratospheric air along the subtropical jet raised tropospheric O3 in early March by approx.40-50 ppbv, especially poleward of approx. 10degN. (4) Influences of lightning and large-scale biomass burning were not strong during this period, in contrast to the situation in Africa and the South Atlantic or locally in Southeast Asia. This work illustrates successes and limitations in approaches to synthesizing disparate information on trace-gas distributions taken from satellite retrieval products and ozonesondes.

Chatfield, R. b.↗
NASA NTRS1983

Latitudinal variation of tropospheric ozone in a photochemical model

A zonally, vertically, and annually averaged numerical model of trace gases in the troposphere is used to examine the variation of ozone as a function of latitude. Processes included in the ozone budget are a source due to downward transport of ozone from the stratosphere, deposition at earth's surface, north-south diffusive transport, and photochemical reactions. Sensitivity of calculated ozone concentrations to the latitude variation and magnitude of the stratospheric source is presented. The model indicates a net photochemical source of ozone in the Northern Hemisphere and a net chemical sink in the tropical latitudes. Calculated variation of ozone concentration with latitude is in qualitative agreement with observations.

Hameed, S.↗
NASA NTRS1998

Global tropospheric ozone investigations

Ozone (O3) is one of the most important trace gases in the troposphere, and it is responsible for influencing many critical chemical and radiative processes. Ozone contributes to the formation of the hydroxyl radical (OH), which is central to most chemical reactions in the lower atmosphere, and it absorbs UV, visible, and infrared radiation which affects the energy budget and atmospheric temperatures. In addition, O3 can be used as a tracer of atmospheric pollution and stratosphere troposphere exchange. At elevated concentrations, O3 can also produce detrimental biological and human health effects. The US National Research Council (NRC) Board on Sustainable Development reviewed the US Global Change Research Program (USGCRP) [NRC, 1995], and it identified tropospheric chemistry as one of the high priority areas for the USGCRP in the next decade. The NRC identified the following specific challenges in tropospheric chemistry. Although we understand the reason for the high levels of 03 over several regions of the world, we need to better establish the distribution of O3 in the troposphere in order to document and understand the changes in the abundance of global tropospheric O3. This information is needed to quantify the contribution of O3 to the Earth' s radiative balance and to understand potential impacts on the health of the biosphere. Having recognized the importance of particles in the chemistry of the stratosphere, we must determine how aerosols and clouds affect the chemical processes in the troposphere. This understanding is essential to predict the chemical composition of the atmosphere and to assess the resulting forcing effects in the climate system. We must determine if the self-cleansing chemistry of the atmosphere is changing as a result of human activities. This information is required to predict the rate at which pollutants are removed from the atmosphere. Over nearly two decades, airborne Differential Absorption Lidar (DIAL) systems have been used in over fifteen major field experiments conducted all over the world to address important atmospheric processes affecting the amount and distribution of 03 and aerosols across the troposphere. This paper discusses some of these wide-ranging field experiments and their results and presents a direction for future global studies of O3 and aerosols from space.

Browell, Edward V.↗
NASA NTRS1990

An assessment of potential impact of alternative fluorocarbons on tropospheric ozone

While the chlorofuorocarbons (CFCs) such as CFC-11 (CFCl3) and CFC-12 (CF2Cl2) are chemically inert in the troposphere, the hydrogen-containing halocarbons being considered as their replacements can, to a large extent, be removed in the troposphere by the HO radical. These alternative halocarbons include the hydrochlorofluorocarbons (HCFCs) 123 (CF3CHCl2), 141b (CFCl2CH3), 142b (CF2ClCH3), 22 (CHF2Cl), and 124 (CF3CHFCl) and the hydrofluorocarbons (HCFs) 134a (CF3CH2F), 152a (CHF2CH3) and 125 (CF3CHF2). Listed are the rate constants (k) for the HO radical reaction of these compounds and their estimated chemical lifetimes in the troposphere. In this table, values of the lifetimes of these selected HCFCs and HCFs are seen to vary by more than a factor of more than ten ranging from 1.6 years for HFC 152a and HCFC 125 to as long as 28 years for HFC 125. Clearly, from the standpoint of avoiding or minimizing impact on stratospheric O3, those halocarbons with short tropospheric lifetimes are the desirable alternates. However, potential environmental consequences of their degradation in the troposphere should be assessed and taken into account in the selection process.

Niki, Hiromi↗
NASA NTRS1992

Distribution of tropospheric ozone at Brazzaville, Congo, determined from ozonesonde measurements

An analysis of 33 ozonesonde launches in Brazzaville, Congo (4 deg S, 15 deg E), between June 1990 and May 1991 is presented. The data indicate highest tropospheric amounts between June and early October, coincident with the dry season and with the presence of enhanced widespread biomass burning. The seasonal cycle of ozone derived from the ozonesonde measurements is in good agreement with the climatological seasonal cycle inferred from the use of satellite data amd both seasonal cycles peak in September. Averaged throughout the year, the integrated amount of ozone derived from the ozonesondes is 44 Dobson units (DU) and is 39 DU using the satellite data. Within the troposphere the highest partial pressures are generally found at pressure levels near 700 mbar (about 3 km). Using simultaneous ozonesonde data from Ascension Island (8 deg S, 15 deg W), examples are presented illustrating that differences in the troposphere are primarily responsible for the observed spatial gradients of total ozone observed by TOMS.

Cros, Bernard↗
NASA NTRS1993

Upper tropospheric ozone production following mesoscale convection during STEP/EMEX

The chemistry and dynamics of a convective system observed on February 2, 1987 in the EMEX and STEP campaigns are analyzed. Chemical and thermodynamic profiles in undisturbed air near the EMEX 9 system indicate that the troposphere was well mixed by previous convection. As a consequence there was little direct transport from the boundary layer to the upper troposphere and air transported upward was detrained throughout the middle and upper troposphere. There was minimal effect on O3 production. Other convective complexes located 800-900 km upstream produced greater perturbations on trace gas profile immediately below the tropopause. Ozone production was reduced by about 0.25 ppbv/d at these altitudes, representing a reduction in P(O3) of 15-20 percent over the column from 14.5 to 17 km. P(O3) from 12 to 17 km in a region distant from active convection and subject to lightning was 2-3 times higher than it would have been without lightning.

Pickering, Kenneth E.↗
NASA NTRS1991

Tropospheric ozone and aerosols measured by airborne lidar during the 1988 Arctic boundary layer experiment

Ozone (O3) and aerosol distributions were measured from an aircraft using a differential absorption lidar (DIAL) system as part of the 1988 NASA Global Tropospheric Experiment - Arctic Boundary Layer Experiment (ABLE-3A) to study the sources and sinks of gases and aerosols over the tundra regions of Alaska during the summer. The tropospheric O3 budget over the Arctic was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were usually correlated with descending air from the upper troposphere or lower stratosphere. Several cases of continental polar air masses were examined during the experiment. The aerosol scattering associated with these air masses was very low, and the atmospheric distribution of aerosols was quite homogeneous for those air masses that had been transported over the ice for greater than or = 3 days. The transition in O3 and aerosol distributions from tundra to marine conditions was examined several times. The aerosol data clearly show an abrupt change in aerosol scattering properties within the mixed layer from lower values over the tundra to generally higher values over the water. The distinct differences in the heights of the mixed layers in the two regions was also readily apparent. Several cases of enhanced O3 were observed during ABLE-3 in conjunction with enhanced aerosol scattering in layers in the free atmosphere. Examples are presented of the large scale variations of O3 and aerosols observed with the airborne lidar system from near the surface to above the tropopause over the Arctic during ABLE-3.

Browell, Edward V.↗
NASA NTRS1994

Summertime tropospheric ozone distributions over central and eastern Canada

Ozone measurements were obtained between the surface and the 6-km altitude on aircraft flights over central and eastern Canada during the summer 1990 NASA Global Tropospheric Experiment Arctic Boundary Layer Expedition (GTE/ABLE 3B). Tropospheric O3 budgets for these regions were observed to be highly variable and significantly impacted by long-range transport and regional scale air mass modification processes. For example, integrated O3 abundance below 5-km altitude averaged 40% and 30% greater in air masses influenced by anthropogenic sources and biomass burning, respectively, than in background (polar) air. Conversely, aged air transported from subtropical areas of the Pacific at times reduced O3 abundance in this height interval by up to 20%. Though intrusion of anthropogenic air was infrequent during the experiment period, the influence of biomass-burning emissions was particularly notable as two thirds of the flights sampled air influenced by plumes from fires burning in Alaska and western Canada. The impinging pollution, both natural and anthropogenic, not only elevated O3 levels directly but also was a source of reactive nitrogen (and nonmethane hydrocarbons) which generally increases the tropospheric lifetime of O3 via moderation of photochemical destruction rates.

Anderson, B. E.↗
NASA NTRS1992

Tropospheric ozone and aerosol observations - The Alaskan Arctic

This paper discusses in situ measurements of O3, aerosol number density, and aerosol size obtained during NASA Arctic Boundary Layer Expedition aircraft flights over the Alaskan Arctic region. The major source of summer O3 for the troposphere in the intrusion of stratospheric air and subsequent transport to lower altitudes. Photochemistry of mixed layer emissions and O3 transported from high northern latitude urban/industrialized areas do not appear to play major roles as sources of O3 for the Alaska region. O3 gradients reflect the loss at the surface and supply from the stratosphere. Free tropospheric O3 averaged 74 ppbv compared to 32 ppbv for the mixed layer. O3 loss mechanisms are a combination of the destruction via photochemistry, chemical reaction with surface emissions, and direct loss through deposition to the surface. The boreal forest in the most efficient of the O3 sinks and has the largest increase in aerosol number density relative to the free troposphere.

Gregory, Gerald L.↗